Like so many of these saints, Raymund wanted to hang around the monastery, reading and praying. Sometimes, if he felt like stretching his legs, he'd go evangelize among the Moors and Jews of Spain, or he'd contend with the heretics. It was the twelfth and thirteenth centuries, so there were still plenty of Moors, Jews, and heretics in Spain, and unlike his Dominican heirs, Raymund didn't light his theological opponents on fire.
He did however get called away from these joyous to be the confessor for Pope Gregory IX. Once Ray was in Rome, Pope Gregory decided to take advantage of his doctorates in canon and civil law by asking him to codify all the papal decrees. The resultant law code served the Vatican (and the rest of the Catholic world) for centuries.
Raymund tried to return to the quiet life, but the people of Aragone tried to make him their bishop. He dodged that bullet, but was selected as the third leader of the Dominican Order. He wrote a new constitution for the Order, putting in a clause which allows the leader of the Order to retire at 65 if he wishes. Raymund wished so, and did so, promptly after his 65th birthday. I like a guy who uses his constitutional powers to get out of a job, especially if he then goes out to plant churches and monasteries throughout Spain.