Stiffness tuning is crucial in developing many advanced engineering systems such as morphing aircraft, soft robotics, etc. Achieving a significant stiffness change while maintaining a high load-bearing capacity in compression is a challenging task. This study addressed this challenge by exploiting the in-plane buckling and bistability of asymmetric carbon fiber composite laminates. Due to the inverted curvatures of these laminates at their two stable states, they showed two distinct in-plane compression behaviors—stiff response where the laminate behaved like a thin curved column (with a stiffness coefficient near 68 N mm−1), and compliant response where the laminate acted like a soft non-linear spring (with stiffness near 0.7 N mm−1). As a result, a simple snap-though between these two stable states offered a significant stiffness change, with a high/low stiffness ratio of ≈97. By using extensive finite element simulations, experimentation, and a semi-empirical curved plate buckling model, this study examined the mechanics underpinning the laminate’s 3-step buckling and the influences of asymmetric boundary contacts with friction. Additionally, three strategies to enhance the laminate’s performance—adjusting the aspect ratio, applying lateral loads, and parallel stacking were examined. It also demonstrated cellular structure concepts using these bistable laminates. Remarkably, by simply adding a small lateral in-plane force (e.g., a rubber band), one could substantially increase the stiffness ratio of the composite laminates to ≈200 and load-bearing capacity at the stiff configuration, outperforming the state-of-art variable stiffness methods.