After a brief stint teaching for the Lazarists at the minor seminary in Soissons, he abandoned his religious aspirations and discovered his passion for pedagogy.
[2] In Paris, Bailly de Surcy established a residence for provincial students, providing accommodation and spiritual guidance.
In 1819, he founded a family-style boarding school that catered to Catholic families, eventually moving the institution to Rue de l'Estrapade.
[2] In 1833, he acquired a printing press on Place de la Sorbonne and later founded the Catholic newspaper L'Univers.
Although initially successful, the paper faced financial difficulties, leading to its eventual takeover by Charles de Montalembert and its editorial leadership passing to Louis Veuillot.