Metal-organic frameworks (MOFs) have intriguing and tunable photophysical properties owing to predesignable structures from well-defined metal and/or organic chromophores. We propose a one-pot two-step assembly strategy for engineering dual-functional coordination interspace where two kinds of organic linkers are segregated in predefined positions. This design endows the three-dimensional coordination framework with unidirectional deformation character, leading to an orientation-dependent and pressure-responsive photoluminescence color change. For the first time, unique piezofluorochromic anisotropism is achieved and can be accumulated stepwise and visualized by a metal-organic framework single crystal, providing a basic model for application in stimuli-responsive photoluminescence sensing, barcoding, signal switching, harvesting, and magnifying micro-devices.