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In nature, structural and functional materials often form programmed three-dimensional (3D) assembly to perform daily functions, inspiring researchers to engineer multifunctional 3D structures. Despite much progress, a general method to fabricate and assemble a broad range of materials into functional 3D objects remains limited. Herein, to bridge the gap, we demonstrate a freeform multimaterial assembly process (FMAP) by integrating 3D printing (fused filament fabrication (FFF), direct ink writing (DIW)) with freeform laser induction (FLI). 3D printing performs the 3D structural material assembly, while FLI fabricates the functional materials in predesigned 3D space by synergistic, programmed control. This paper showcases the versatility of FMAP in spatially fabricating various types of functional materials (metals, semiconductors) within 3D structures for applications in crossbar circuits for LED display, a strain sensor for multifunctional springs and haptic manipulators, a UV sensor, a 3D electromagnet as a magnetic encoder, capacitive sensors for human machine interface, and an integrated microfluidic reactor with a built-in Joule heater for nanomaterial synthesis. This success underscores the potential of FMAP to redefine 3D printing and FLI for programmed multimaterial assembly.