Designing 3D hydrogels with user-defined geometries can facilitate a variety of basic research in biomaterials science and tissue engineering. In their article on page 4799, R.Liska, X.-H. Qin, and coworkers report the direct assembly of 3D hydrogel structures with free-transport properties via two-photon thiolene lithography. This study reports the first biomacromolecule with pendant, low cytotoxic vinyl ester groups and subsequent copolymerization with free cysteines donated by reduced albumin. The cover image shows a 3D hydrogel construct (480 × 580 × 75 μm3) consisting of three layers of packed cylinders with a hexagonal arrangement. This method may lead researchers to better understand how cells detect and respond to their micro-environmental signals.