Half metals, which are amenable to perfect spin filtering, can be utilized for high-magnetoresistive devices. However, available half metals are very limited. Here, we demonstrate that materials with intrinsic spin-valley-mismatched (SVM) states can be used to block charge transport, resembling half metals and leading to giant tunneling magnetoresistance. As an example, by using first-principles transport calculations, we show that ferromagnetic 1T-VSe_{2}, 1T-VS_{2}, and 2H-VS_{2} are such spin-valley-mismatched metals, and giant magnetoresistance of more than 99% can be realized in spin-valve van der Waals (vdW) junctions using these metals as electrodes. Owing to the intrinsic mismatch of spin states, the central-layer materials for the vdW junctions can be arbitrary nonmagnetic materials, in principle. Our research provides clear physical insights into the mechanism for high magnetoresistance and opens new avenues for the search and design of high-magnetoresistance devices.