In the past decades, ionic liquids (ILs) have garnered a lot of attention especially in the field of green chemistry due to their unique properties which help to solve the problems posed by organic solvents. Interestingly, their applications are not limited to that only as ILs have the potential to become alternative templates in the development of mesoporous silica nanoparticles (MSNs). This work reported the usage of a series of pyridinium ILs as template in the synthesis of monodispersed mesoporous silica nanosphere (MNSs) via two methods. Both syntheses utilize triethanolamine (TEA) as the base catalyst where in one method the TEA undergoes pre-treatment process while the other did not. Besides that, the effects of pyridinium ILs alkyl chain length were also investigated. MNSs generated via both methods exhibit spherical morphology and decreasing average particles size with increasing alkyl chain length of pyridinium ILs. The MNSs porosity were further analyzed through nitrogen sorption analysis where the surface area were in between 71.85 and 525.02 m 2 g −1 and the pore volume was up to 1 cm 3 g −1 .