Laser direct write (LDW) is a widely regarded 3D printing technology with nearly arbitrarily free 3D writing capabilities. Using ultrafast lasers, high fabrication resolution due to multi-photon absorption processes and reduced heat accumulation effects are key advantages. Using femtosecond laser direct write (fs-LDW) with protein precursor, 3D proteinaceous microstructures for various biomimetic and biomedical applications can be fabricated. 3D printing of protein allows the fabrication of soft biocompatible microstructures that retain the native protein function and respond to pH-actuation. To avoid undesired effects from leaching of photoactivators after fabrication, pure protein precursor can be used, wherein protein molecules both fulfill activator and monomer roles. Though the fabrication mechanism is not yet fully understood, we showed in the recent years that certain amino acids are beneficial to the fabrication process and that chemical crosslinking are induced by fs-LDW. We will present an overview of the field and show our recent research interest of free-form fabrication. Due to the diversity of the biomacromolecule protein, this technology is promising the fabrication of biomimetic 3D microstructures, with applications in microfluidics and soft robotics.