The mineral-organo composites control the speciation, mobility and bioavailability of heavy metals in soils and sediments by surface adsorption and precipitation. The dynamic changes of soil mineral, organic matter and their associations under redox, aging and microbial activities further complicate the fate of heavy metals. Over the past decades, the wide application of advanced instrumental techniques and modelling has largely extended our understanding on heavy metal behavior within mineral-organo assemblages. In this review, we provide a comprehensive summary of recent progress on heavy metal immobilization by mineral-humic and mineral-microbial composites, with a special focus on the interfacial reaction mechanisms of heavy metal adsorption. The impacts of redox and aging conditions on heavy metal speciations and associations with mineral-organo complexes are discussed. The modelling of heavy metals adsorption and desorption onto synthetic mineral-organo composites and natural soils and sediments are also critically reviewed. Future challenges and prospects in the mineral-organo interface are outlined. More in-depth investigations are warranted, especially on the function and contribution of microorganisms in the immobilization of heavy metals at the complex mineral-organo interface. It has become imperative to use the state-of-the-art methodologies to characterize the interface and develop in situ analytical techniques in future studies.