Pressure–compression asymmetry is a subject of present curiosity in nanostructures, particularly in pressure engineering. Herein, we report a novel on-chip microelectromechanical system (MEMS) that may understand in situ quantitative mechanical testing of nanostructures underneath pressure–compression features. The mechanical properties of three sorts of nanostructures fabricated by centered ion beam (FIB) methods have been systematically investigated with the introduced on-chip testing system. The outcomes declare that each Pt nanopillars and C nanowires exhibit plastic deformation conduct underneath pressure testing, with common Younger’s moduli of 70.06 GPa and 58.32 GPa, respectively. Nevertheless, the mechanical deformation mechanisms of the 2 nanostructures modified in compression checks. The Pt nanopillar exhibited in-plane buckling conduct, whereas the C nanowire displayed 3D twisting conduct with a most pressure of 25.47%, which is much higher than the tensile pressure. Furthermore, uneven conduct was additionally noticed within the C nanospring throughout 5 loading–unloading pressure–compression deformation checks. This work gives a novel perception into the uneven mechanical properties of nanostructures, with potential purposes in nanotechnology analysis.