The hetero-/homogenous combustion-based HCCI (homogeneous charge compression ignition) of fuel lean methane-air mixtures over alumina-supported platinum catalysts was investigated experimentally and numerically in free-piston micro-engines without ignition sources. Single-shot experiments were carried out in the purely homogeneous and coupled hetero-/homogeneous combustion modes, involved temperature measurements, capturing the visible combustion image sequences, exhaust gas analysis, and the physicochemical characterization of catalysts. Simulations were performed with a two-dimensional transient model that includes detailed hetero-/homogeneous chemistry and transport, leakage, and free-piston motion to gain physical insight and to explore the hetero-/homogeneous combustion characteristics. The micro-engine performance concerning combustion efficiency, mass loss, energy density, and free-piston dynamics was investigated. The results reveal that both purely homogeneous and coupled hetero-/homogeneous combustion of methane-air mixtures in a narrow cylinder with a diameter of 3 mm and a height of approximately 0.3 mm are possible. The coupled hetero-/homogeneous mode can not only significantly improve the combustion efficiency, in-cylinder temperature and pressure, output power and energy density, but also reduce the mass loss because of its lower compression ratio and less time spent around TDC (top dead center) and during the expansion stroke, indicating that this coupled mode is a promising combustion scheme for micro-engine. Heat losses result in higher mass losses. Heterogeneous reactions cause earlier ignition, which is very favorable for the micro-device. (C) 2016 Elsevier Ltd. All rights reserved.