alignment and excellent interfacial contact. [8] By contrast, carefully engineering the nanostructure of Ta 3 N 5 with good crystallinity to shorten the migration length of charge carriers and provide more reactive sites may open up new opportunities for efficient water splitting.Over the past decade, enlightened by the breakthrough of graphene, [9] 2D nanomaterials have attracted increasing research-attention in the field of energy storage and conversion because they possess advantages of large specific surface area, high ratio of surface atoms, and facile charge transport behaviour. [10] However, the amount of catalytic active sites in 2D nanosheets is still confined due to the limited boundaries and exposed edges. It has been demonstrated that constructing 2D nanosheets with abundant and well-distributed pores, or namely, nanomeshes, can solve this problem and greatly improve the catalytic performance. [11] Unfortunately, the construction of ultrathin nanomeshes is mainly limited to the materials with layered structure, such as graphene, boron nitride, and layered double hydroxides. [11a,12] The fabrication of ultrathin nanomeshes for the nonlayered and transition metalbased materials such as Ta 3 N 5 with potentially high catalytic activity is of great challenge.Herein, we innovatively synthesize ultrathin single-crystalline Ta 3 N 5 nanomeshes using graphene oxide (GO) nanosheets as a 2D template. Remarkably, the obtained 2D Ta 3 N 5 nanomeshes with a lateral size of several micrometres and an average thickness of ≈2 nm show large aspect ratios, high specific surface area (284.6 m 2 g −1 ), and excellent crystallinity. The interplane pores provide numerous new active edges which can greatly speed up mass transfer and charge migration. Furthermore, the high crystallinity is also beneficial for charge separation. By loading 1 wt% of Pt as cocatalysts, the Ta 3 N 5 nanomeshes exhibit over tenfold improvement of solar hydrogen production when compared to its bulk counterpart. [1b] This work provides a novel strategy for designing 2D ultrathin nanomesh structures for nonlayered materials with improved photocatalytic activity.As shown in Figure 1, Ta 3 N 5 nanomeshes were synthesized via a bottom-up process using GO as a template. First, a thin layer of amorphous Ta-aquo-complex was uniformly deposited on the GO sheets by a homogeneous hydrolysis process of TaCl 5 , yielding GO/Ta-aquo-complex composite nanosheets. Then, the GO template was removed using a calcination procedure to obtain 2D-TaO x nanosheets. Finally, the Tantalum nitride (Ta 3 N 5 ) with a suitable bandgap (≈2 eV) is regarded as one of the most promising photocatalysts for efficient solar energy harvesting and conversion. However, Ta 3 N 5 suffers from low hydrogen production activity due to the low carrier mobility and fast carrier recombination. Thus, the design of Ta ) and excellent crystallinity by an innovative bottom-up graphene oxide templated strategy. The resulting Ta 3 N 5 nanomeshes demonstrate drastically improved electron trans...