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Integration of diverse materials into 3D ordered structures is urgently required for advanced manufacture owing to increase in demand for high-performance products. Most additive manufacturing techniques mainly focus on simply combining different equipment, while interfacial binding of distinctive materials remains a fundamental problem. Increasing studies on macroscopic supramolecular assembly (MSA) have revealed efficient interfacial interactions based on multivalency of supramolecular interactions facilitated by a "flexible spacing coating." To demonstrate facile fabrication of 3D heterogeneous ordered structures, the combination of MSA and magnetic field-assisted alignment has been developed as a new methodology for in situ integration of a wide range of materials, including elastomer, resin, plastics, metal, and quartz glass, with modulus ranging from tens of MPa to over 70 GPa. Assembly of single material, coassembly of two to four distinctive materials, and 3D alignment of "bridge-like" and "cross-stacked" heterogeneous structures are demonstrated. This methodology has provided a new solution to mild and efficient assembly of multiple materials at the macroscopic scale, which holds promise for advanced fabrication in fields of tissue engineering, electronic devices, and actuators. Additive manufacture, especially three dimentional (3D) printing, is a revolutionary concept with applications in diverse fields. [1-4] Owing to the increase in demand for differently processed materials with multiple functions for advanced applications such as tissue engineering, the research of additive manufacture is facing new challenges of integrating multicomponents into one entity with high-performance or desired functions. [5,6] For example, ex situ cell growth and tissue formation require complex 3D microenvironments consisting of

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