The Greater Caucasus (GC) fold-and-thrust belt lies on the southern deformed edge of the Scythian Platform (SP) and results from the Cenoozoic structural inversion of a deep marine Mesozoic basin in response to the northward displacement of the Transcaucasus (lying south of the GC subsequent to the Arabia-Eurasia collision. A review of existing and newly acquired data has allowed a reconstruction of the GC history through the Mesozoic and Cenozoic eras. In Permo(?)-Triassic times, rifting developed along at least the northern part of the belt. Structural inversion of the basin occurred during the Late Triassic corresponding to the Eo-Cimmerian orogeny, documented SE of the GC and probably linked to the accretion of what are now Iranian terranes along the continental margin. Renewed development of extensional basin formation in the area of the present-day GC began in Sinemurian-Pliensbachian times with rift activity encompassing the Mid-Jurassic. Rifting led to extreme thinning of the underlying continental crust by the Aalenian and concomitant extrusion of mid-ocean ridge basalt lavas. A Bathonian unconformity is observed on both sides of the basin and may either correspond to the end of active rifting and the onset of post-rift basin development or be the record of collision further south along the former Mesozoic active margin. The post-rift phase began with deposition of Late Jurassic platform-type sediments onto the margins and a flysch-like unit in its deeper part, which has transgressed the basin during the Cretaceous and Early Cenozoic. An initial phase of shortening occurred in the Late Eocene under a NE-SW compressional stress regime. A second shortening event that began in the Mid-Miocene (Sarmatian), accompanied by significant uplift of the belt, continues at present. It is related to the final collision of Arabia with Eurasia and led to the development of the present-day south-vergent GC fold-and-thrust belt. Some north-vergent retrothrusts are present in the western GC and a few more in the eastern GC, where a fan-shaped belt can be observed. The mechanisms responsible for the large-scale structure of the belt remain a matter of debate because the deep crustal structure of the GC is not well known. Some (mainly Russian) geoscientists have argued that the GC is an inverted basin squeezed between deep (near)-vertical faults representing the boundaries between the GC and the SP to the north and the GC and the Transcaucasus to the south. Another model, supported in part by the distribution of earthquake hypocentres, proposes the existence of south-vergent thrusts flattening at depth, along which the Transcaucasus plunges beneath the GC and the SP. In this model, a thick-skinned mode of deformation prevailed in the central part of the GC whereas the western and eastern parts display the attributes of thin-skinned fold-and-thrust belts, although, in general, the two styles of deformation coexist along the belt. The present-day high elevation observed only in the central part of the belt would have resulted from the delamination of a lithospheric root.