Due to the increasingly polluted environment and the gradual depletion of fossil fuel reserves, the development of renewable technologies for environmental remediation and energy production is highly desirable. Over the past decades, oxide-based semiconductor photocatalysis has attracted much attention. On various frontiers for efficient photocatalysis, surface-tuning strategies for synthesis and modification of oxides on the nanometer scale have progressed at a fast pace. Hence, it is of significance to review recent advances in the development of surface tuning for oxide-based nanomaterials as activity-enhanced photocatalysts. In this review, special emphases, especially for recent advances in our group, are given to surface tuning of novel nanocrystallites for high thermal stability, hierarchical structure assembly, heterojunctional nanocomposites and high-energy-facet exposure, along with effective testing tools for photogenerated charge properties at the surfaces and/or interfaces. This is of great significance for fields related to energy and environment from scientific and engineering viewpoints.