The Chronicle of Alberic de Trois-Fontaines names "Guilelmum et Raymundum" as the two sons of "Guilelmi…Tolose comitis" and his wife "Alymodis multinuba". "Wilelmo…Raimundo…Ugoni" are named as sons of "Pontio [comite Tolosano]" in a charter dated 9 Jun 1063.
Comte de Rouergue, de Nîmes et de Narbonne, presumably resulting from an agreement with his brother to partition their father's territories following his death in 1060. "Raimundum comitem de Rutenis, filium Almodis" and "Guifredum archiepiscopum de Narbona, filium Guille comitissæ" confirmed an agreement by charter dated to [1066], confirmed by "uxorem suam comitissam". "Raimundus comes Rutenensis et Nemosensis, Narbonensiumque filius meus" joined "Almodis comitissa" in a transaction with Cluny for the soul of "Poncii comitis" dated 15 Dec 1066. "Raimundi comitis Rutenensis…" subscribed the charter dated 7 Sep 1071 which records an agreement between "Wuiellmum Tolosanum comitem" and "Raimundum comitem Barchinonensem et Carchanonensem et Raimundem filium eius" settling their dispute about "castello de Laurago" [Lauragais]. "Rogerius comes Fuxensis et coniux mea Sicardis comitissa" donated property to Saint-Pons de Thomières by charter dated to [1074], subscribed by "domni G. comitis Tolosani et domni Raymundi fratris eius comitis Ruthenæ". A charter dated 27 Jun 1078 records a hearing held by "Raymundo Ruthenensium comiti et Biterrensium vicecomitissæ Hermengardi" relating to a claim by "Petrus…Bermundi filius". "Guillelmus Tolonanensium, Albensium seu Caturcensium, Lutevensium, Petragorensium, Carcassonensium, Aginnensium necne Astarachensium comes et dux…cum uxore mea…Emma" confirmed donations by "proavuo…meo Pontio Aquitanorum duce" to Saint-Pons de Thomières by charter dated 16 Jun 1080, signed by "Regimundus comes frater eius, Bertrandus comes nepos Willelmi et filius Raimundi, Guillelmi de Rehenti, Ademari vicecomitis…". He took an active part in the crusade against the Moors in Spain. "Raymundus comes Rothenensis" abandoned rights in favour of the church of Béziers by charter dated 1084, signed by "…Guillelmi de Sabrano…". "Raymundus Ruthenensis, Gabalitanus, Ucetiensis, Nemausensis, Agathensis, Biterrensis necnon Narbonensis comes" confirmed the foundation of the abbey of Saint-Pons de Thomières by "proavo…meo Pontio Aquitanorum magno duce vel principe" by charter dated 1085.
He succeeded his brother in 1094 as RAYMOND IV "de Saint-Gilles" Comte de Toulouse. "Raimundus comes Tolosanæ, dux Narbonæ, marchio Provinciæ" donated property to Saint-André d´Avignon by charter dated 1088 (which presumably should be redated to after 1094), signed by "…Guillelmus de Sabrano, Alisiardus de Usetico, Rostagnus de Posqueriis, Gibellinus de Sabrano…". A bull of Pope Urban II dated 18 Feb 1095 announced that "Raimundus Tolosanus comes…cum uxore sua Hervira et filio Bertranno" abandoned his rights to altar offerings at the monastery of Saint-Gilles. Presumably Comte Raymond's epithet "de Saint-Gilles" is attributable to his continuing public support for this monastery rather than use of a title such as "Comte de Saint-Gilles" before succeeding his brother in Toulouse. He was the first noble to answer the call of Pope Urban IV for a crusade to relieve Jerusalem from occupation by the Muslim Arabs, asking to join the expedition 1 Dec 1095 only days after the Pope's rallying speech at the Council of Clermont.
He succeeded as Marquis de Provence, no doubt after the death of Bernard [II] Comte de Provence in [1090/94] although the precise process by which this succession occurred has not yet been identified. "Raimundus…comes et Provincie marchio" donated property to Saint-Victor, Marseille by charter dated 28 Jul 1094, also confirming donations by "Dulcis comitissa", signed by "Alvira comitissa". A bull of Pope Urban II dated 22 Jul 1096 confirmed the rights of the monastery of Saint-André near Avignon after its abandonment by "comes Nimirum Tholosanorum ac Ruthenensium et marchio Provintie Raimundus". In Jul 1096, Comte Raymond transferred many of his possessions to the monastery of Saint-Gilles. He left on crusade in Oct 1096, leaving the government of Toulouse in the hands of his older son Bertrand (not named but referred to as "naturali cuidam filio suo comitatu quem regebat relicto"). Comte Raymond never returned to France. While crossing Byzantine territory, his army attacked Roussa in Thrace, but was defeated and dispersed by the Imperial army. He played a decisive role in the capture of Antioch 28 Jun 1098 after a siege lasting eight months. The leaders of the crusade disagreed about who should control Antioch. After Comte Raymond finally marched south in Jan 1099 to continue the crusade. Bohémond of Apulia remained in possession of Antioch. Comte Raymond tried unsuccessfully to be accepted as overall leader of the crusade, but in Jul 1099 refused to be considered as a candidate to be "King of Jerusalem" knowing that he did not have enough support among the crusaders. After the election as leader of his rival Godefroi de Bouillon 22 Jul 1099, Comte Raymond left Jerusalem for Jericho. His objective was to create his own principality in central Syria. He established his household at Lattakia. The second wave of the First Crusade, Lombards who had left Italy under Alberto Conte di Biandrate in Sep 1100 and the French under Etienne Comte de Bourgogne who left in Spring 1101, appointed Comte Raymond as their leader when they arrived at Constantinople, where he was staying during the winter of 1100/01 as the guest of Emperor Alexios. After the combined armies left Constantinople in May 1101, they captured Ankara from the Seljuk Turks 23 Jun 1101 but were scattered after their defeat by the Turks at Mersivan. Comte Raymond returned to Constantinople, left by ship for Lattakia, but in early 1102 was arrested in Tarsus for having "betrayed Christendom" and taken to Tancred Regent of Antioch who released him only after he swore an oath not to interfere further in affairs in Syria, In compliance, he evacuated his garrison from Lattakieh, which was besieged by Tancred in early Spring 1102. He gained a notable victory against the Turks outside Tripoli in 1102, constructed the castle of Mount Pèlerin near Tripoli in 1103/04, and laid siege to the town itself. He died during the course of the siege, his death being recorded by William of Tyre.
Albert of Aix records that "comes Reimundus" died at "Mons Peregrinorum", which he had built, in February "post Purificationem sanctæ Mariæ" and was buried there. Bar Hebræus records the death in A.H. 499 (1105/06) of "Hisn Sandjil", ten days after falling from a roof which had been set alight by "Abou-Ali Ibn Ammar, souverain de Tripoli", and his burial in Jerusalem. 1
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