Combination of the advantages of the surface-initiated atom transfer radical polymerization (SI-ATRP) and template-based techniques, the SI-ATRP from colloidal templates approach could be applied to fabricate the controllable-structured polymeric nanocapsules. The different crosslinking techniques, such as chemical crosslinking, ultraviolet (UV)-induced photo-crosslinking, and one-pot surface-initiated atom transfer radical crosslinking copolymerization (SI-ATRCP), for the controllable-structured crosslinked polymeric nanocapsules based on the SI-ATRP from colloidal templates strategy were reviewed. The controlling and tailoring on the size, crosslinking degree, and the surface properties of the polymeric nanocapsules was emphasized. And the stimuli-responsive properties and application in controlled release were also mentioned.