Mesoporous silica nanoparticles (MSNs) have been demonstrated as a promising candidate in drug delivery applications. With the ambition of enhancing their drug loading capacity and controlled release, in this innovative study, MSNs were tailored with polyamidoamine (PAMAM) dendrimers thereby exerting advantageous properties onto the surface of the nanoplatforms. MSNs were prepared by Stöber’s method, sequentially functionalised by amine groups, and respectively grafted with PAMAMs layer-by-layer. Morphology and characterisation of the nanoparticles were carried out through transmission electron microscopy, dynamic light scattering, thermogravimetric analysis, and Fourier-transform infrared spectroscopy. Ninhydrin assay and zeta potential analysis were further employed to investigate the amine-modified nanomaterials. The drug loading and release profiles of particles were also studied. As a result, PAMAM-grafted MSNs, with the highest hydrodynamic size of 185.3 nm, exhibited high encapsulation efficiency (85.8%) and controlled release ability compared to conventional MSNs, suggesting that PAMAM-grafted MSNs would be a promising drug delivery system.