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Crystalline linear polyethyleneimine (LPEI) is a fascinating polymer that can be used as a catalyst, template and scaffold in order to direct the formation of silica with controllable compositions and spatial structures under mild conditions. Considering the crystallization and assembly of LPEI is temperature-dependent, we adopted different accelerated cooling processes of a hot aqueous solution of LPEI in order to modulate the LPEI crystalline aggregates. We then used them in the hydrolytic condensation of alkoxysilane. A series of silica with nanofibrils, nanotubes and nanowire-based structures were achieved simply by the LPEI aggregates which were pre-formed in defined cooling processes. These specific one-dimensional nanoscale structures assembled into microscale fibers-, sheet- and platelet-like coalescences. Furthermore, the deposition kinetics was also researched by the combination of other characterizations (e.g., pH measurement, 29Si MAS NMR). As a preliminary application, the hybrids of LPEI@SiO2 were used not only as an agent for reducing PtCl4 2- into Pt but also as host for loading Pt nanoparticles. The Pt-loaded silica showed good catalytic properties in the reduction of Rhodamine B by dimethylaminoborane (DMAB) [ABSTRACT FROM AUTHOR]