Caloric cooling offers a promising solid-state alternative to conventional refrigeration. A traditional strategy to enhance cooling performance is increasing disorder-related configurational entropy change, which is a phenomenological approach and sometimes fails. Here, we establish a unified phonon-entropy framework applicable to electrocaloric, magnetocaloric, and mechanocaloric systems. By deriving analytical expressions that link entropy to the phonon density of states and mode-specific entropy, we enable mode-level tuning of caloric performance. Under this framework, we propose three key criteria for high-performance mechanocaloric cooling: high low-frequency phonon density of states, large changes in the product of density of states and mode-specific entropy, and low Young’s modulus. Accordingly, we identify PbO as a superior mechanocaloric material, which exhibits a pressure-induced entropy change nearly 2.7 times greater than TiNi, currently among the best-performing mechanocaloric materials. These findings establish a quantitative framework for phonon-entropy-driven caloric cooling and open other avenues for materials design.

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• Elastocaloric effect
• Electrocaloric effect
• Entropy
• Magnetocaloric effect
• Phonons
• Pressure effects
• Energy materials
• Solid-state refrigeration