Controlling mechanical deformation is one of the state-of-the-art approaches to tune the electronic properties of 2D materials. We report a new mechanism for tuning a phosphorene superlattice with intercalated amphiphiles by its strong anisotropic co-deformation. Anisotropic co-deformation of a phosphorene superlattice is found to follow tunable sinusoidal and Gaussian functions, which exhibit adjustable mechanical actuation, curvature and layer separations. We analysed the controlling mechanism and tuning strategy of co-deformation as a function of amphiphile assembly topology, van der Waals interactions, interlayer separation and global deformation based on Euler-beam theory. Our first-principles calculations demonstrate that the co-deformation mechanism can be used to achieve a theoretical bandgap tunability of 0.7 eV and a transition between direct and indirect bandgaps. The reported tuning mechanisms pave new ways for designing a wide range of tunable functional electronics, sensors and actuators.