In article number 1802319, by Dong-Wan Kim and co-workers, unique 3D architectures of quaternary (Co1−xNix)(S1−yPy)2/Graphene hybrids are developed as high-performance bifunctional electrocatalysts for overall water splitting. By structural and compositional engineering, doughnut-like shaped 3-dimensional architectures of (Co1−xNix)(S1−yPy)2/Graphene are successfully synthesized. (Co1−xNix)(S1−yPy)2/Graphene achieves excellent electrocatalytic hydrogen and oxygen evolution reaction performance as a bifunctional electrocatalyst for overall water splitting.