Three-dimensional (3D) printing or additive manufacturing, as a revolutionary technology for future advanced manufacturing, usually prints parts with poor control of complex gradients for functional applications. We present a single-vat grayscale digital light processing (g-DLP) 3D printing method using grayscale light patterns and a two-stage curing ink to obtain functionally graded materials with the mechanical gradient up to three orders of magnitude and high resolution. To demonstrate the g-DLP, we show the direct fabrication of complex 2D/3D lattices with controlled buckling and deformation sequence, negative Poisson's ratio metamaterial, presurgical models with stiffness variations, composites for 4D printing, and anti-counterfeiting 3D printing.