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Surface engineering of one-dimensional (1D) TiO2-based heterostructures is extremely vital to the development of new photocatalysts with superior performances. Herein, the Al2O3heterojunctions onto TiO2nanofibers were facilely fabricated by a surfactant-free approach, viaemploying graphene oxide (GO) sheets as a reliable catalyst of regulating the growth kinetics of heterojunctions. Through adjusting the GO content, the oxygen-containing functional groups of GO provided nucleation sites of Al2O3species while restricting their growth in the limited space. As a result, the morphology of Al2O3heterojunctions evolved from nanoflakes to nanospikes outside the TiO2nanofibers that served as robust skeletons. Owing to the distinctive morphology and the effective electron transfer pathway, the photocurrent density of the spiny RGO/Al2O3/TiO2nanofibers was 3.5-times higher than that of pure Al2O3/TiO2nanofibers counterparts toward photoelectrochemical reaction under visible-light irradiation. The present work highlights the pivotal role of graphene sheets in controlling the hierarchical growth of TiO2-based heterostructures with tunable morphology and compositions.