LAUSR

Among the different states of matter, liquids have particular advantages in terms of easy handling and recycling, which has been manifested in various chemosynthetic reactions, but remains underexplored in graphene synthesis. This work reports the direct conversion of liquid organic precursor into versatile 3D graphene materials using rapid laser irradiation. The liquid precursor allows for easy fabrication of graphene with significant 3D architectures, including powders, patterned composite structures, and substrate‐free films. Taking advantage of the high compatibility of liquid precursor with a wide range of dopants, the 3D graphene can be further engineered together with various functional components, especially the high loading (≈15 wt.%) and well‐dispersed (an average diameter of less than 50 nm) high‐entropy alloy nanoparticles. Furthermore, combined with the 3D printing strategy, the rapid construction of graphene with complex and accurate 3D shapes is demonstrated via a selective in situ laser transforming (SLT) strategy. With the high structural integrity unachievable by traditional 3D printing methods, the obtained objects show an electrical conductivity of 4380 S m−1 and a compressive modulus of 31.8 MPa. The results reported in this work will open up a new way for the fabrication of functional carbon materials with customizable shapes and components.