Metal aerogels (MAs) are emerging all‐nanometal‐structured self‐standing porous materials featuring exceptional performances in diverse fields. They have recently been adopted as 3D surface‐enhanced Raman scattering (SERS) substrates, while the less utilization of the unique porous structure leads to limited performance. Here, a fascinating compression‐mediated regulation strategy is presented to largely boost the SERS performance of Au–Ag aerogels. By gently pressing, both the density of hot spots and the inter‐ligament distance can be efficiently modulated, thus enabling to flexibly manipulate the SERS properties of MAs. On this basis, a record‐high misfocus tolerance (∼8.8 mm), low detection limit (down to 0.1 nM), high stability (>1 month), reusability, and multiplex detection ability are concurrently realized. This study may point out a new direction for engineering 3D SERS substrates with tunable and exceptional performance.