We describe the synthesis and characterization of wurtzite (Ga 1Àx Zn x )(N 1Àx O x ) nanocrystals with a wide range of compositions and a focus on properties relevant for solar fuel generation. (Ga 1Àx Zn x )(N 1Àx O x ), a solid solution of GaN and ZnO, is an intriguing material because it exhibits composition-dependent visible absorption even though the parent semiconductors absorb in the UV. When functionalized with co-catalysts, (Ga 1Àx Zn x )(N 1Àx O x ) is also capable of water splitting under visible irradiation. Here, we examine the synthesis of (Ga 1Àx Zn x )(N 1Àx O x ) nanocrystals to understand how they form by nitridation of ZnO and ZnGa 2 O 4 nanocrystalline precursors. We find that the ZnO precursor is critical for the formation of crystalline (Ga 1Àx Zn x )(N 1Àx O x ) at 650 C, consistent with a mechanism in which wurtzitenucleates topotactically on wurtzite ZnO at an interface with ZnGa 2 O 4 . Using this information, we expand the range of compositions from previously reported 0.30 # x # 0.87 to include the low-x and high-x ends of the range. The resulting compositions, 0.06 # x # 0.98, constitute the widest range of (Ga 1Àx Zn x )(N 1Àx O x ) compositions obtained by one synthetic method. We then examine how the band gap depends on sample composition and find a minimum of 2.25 eV at x ¼ 0.87, corresponding to a maximum possible solar-to-H 2 power conversion efficiency of 12%. Finally, we examine the photoelectrochemical (PEC) oxidation behavior of thick films of (Ga 1Àx Zn x )(N 1Àx O x ) nanocrystals with x ¼ 0.40, 0.52, and 0.87 under visible illumination. (Ga 1Àx Zn x )(N 1Àx O x ) nanocrystals with x ¼ 0.40 exhibit solar PEC oxidation activity that, while too low for practical applications, is higher than that of bulk (Ga 1Àx Zn x )(N 1Àx O x ) of the same composition. The highest photocurrents are observed at x ¼ 0.52, even though x ¼ 0.87 absorbs more visible light, illustrating that the observed photocurrents are a result of an interplay of multiple parameters which remain to be elucidated. This set of characterizations provides information useful for future studies of composition-dependent PEC properties of nanoscale (Ga 1Àx Zn x )(N 1Àx O x ). † Electronic supplementary information (ESI) available: Fitting of XRD patterns in Fig. 2; TEM images of the samples from Fig. 2; XRD patterns, elemental analysis by ICP-OES, and diffuse reectance spectra of the products from nitridation of the starting mixture with x ¼ 0.78 with varying nitridation time; TEM images of the nitrided products of x ¼ 0.06, 0.24, 0.91, and 0.98; XPS spectra of Zn2p 3/2 , O1s, Ga2p 3/2 , and N1s in samples with several compositions; determination of band gap as a function of composition. See