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 itinerant in England (Pipe Roll, 4 Hen. II, p. 114). John of Salisbury seems to imply (Polycraticus, l. viii. c. 24) that Henry's expedition against Toulouse in 1159 was thought to have been instigated by the chancellor. The taxes imposed to defray its costs were so arranged that a disproportionately heavy share fell on the church; and that Thomas was somehow concerned in this taxation is certain. One of his enemies at a later time said that, ‘having in his hand the sword of the state, he plunged it into the bosom of the church, his mother, when he robbed her of so many thousands for the war of Toulouse;’ while John of Salisbury declared that Thomas was in this matter only ‘a minister of iniquity,’ yielding, under compulsion, to the will of the king. In the war itself the deacon-chancellor figured prominently, at the head of a troop of picked knights, foremost in every fight. When Louis VII came to relieve Toulouse, Thomas vainly urged Henry to continue the siege. When all the great barons refused the task of securing the conquered territory after Henry's withdrawal, Thomas and the constable, Henry of Essex, undertook it, and performed it with signal success. Thomas afterwards defended the Norman border for some months with troops whom he paid at his own cost and commanded in person; he led several forays into France, and once unhorsed a famous French knight in single combat. He negotiated the treaty between Henry and Louis in May 1160. Soon afterwards he incurred Henry's wrath by opposing, though without success, the grant of a papal dispensation for the marriage of Mary, countess of Boulogne and abbess of Romsey.

In May 1162 Thomas returned to England, bringing with him the king's eldest son, of whom he had for some time past had the entire charge, and whose recognition as heir to the crown he had undertaken to procure from the barons. In this he succeeded. Just before leaving Normandy he had learned the king's intention of raising him to the see of Canterbury, vacant since April 1161. The late archbishop, Theobald, had ‘hoped and prayed’ for Thomas as his successor (, Entheticus, ll. 1293–6); but Thomas shrank from accepting the office, avowedly because he knew that Henry's ecclesiastical policy would clash with his own ideas of an archbishop's duty, and that the appointment must lead to a severance of their friendship. A cardinal who was present, however, bade him take the risk, and he consented. The Canterbury chapter, urged by the justiciar in the king's name, elected Thomas archbishop; on 23 May the election was ratified at Westminster by the bishops and clergy of the province; on Saturday, 2 June, he was ordained priest in Canterbury Cathedral by Bishop Walter of Rochester, and next day he was consecrated by the bishop of Winchester [see ]. At the king's request the pope allowed him to send for his pallium instead of fetching it in person; he received it on 10 Aug. Henry had also procured a dispensation for him to retain the seals, but he refused to do so. He kept, however, the archdeaconry of Canterbury till he was forced by the king to resign it in January 1163. Possibly his motive may have been to effect in the archidiaconal administration some reforms which Theobald had desired, but had been unable to accomplish in the absence of the archdeacon, Thomas himself (Materials, v. 9, 10).

The life of the deacon-chancellor, however unclerical, had always been both pious and pure; and he was no sooner consecrated than he became one of the most zealously devout and studious, as well as industrious, of prelates. He seems to have taken St. Anselm [q. v.] for his model; and he made an unsuccessful request for Anselm's canonisation to Alexander III at the council of Tours, May 1163. At a council at Woodstock on 23 July he opposed a project mooted by the king for transferring from the sheriffs' pockets to the royal treasury a certain ‘aid’ which those officers customarily received from their respective shires as a reward for their administrative work. The primate's opposition was based on two grounds: (1) the sheriffs had a claim to the money by long prescription, and as earning it by their services to the people of the shire; (2) the enrolment of these sums among the king's dues would create a written record which would make their payment to him binding on all generations to come, whereas the existing arrangement was merely one of custom, between people and sheriffs, with which neither the king nor the law had anything to do. Thomas thus appears to have stood forth as the champion of justice, first in behalf of the sheriffs, and secondly in behalf of the whole English people. If the case was really as it is represented by contemporary writers, Thomas was right; but the matter is obscure, and all that can be said of it with certainty is that in ‘the first case of any opposition to the king's will in the matter of taxation which is recorded in our national history,’ the opposition was made, and apparently with entire success,