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The Madriu–Perafita–Claror valleys (MPCV) (Eastern Pyrenees, Andorra) were the focus of a multidisciplinary microregional landscape research project that aimed to study the long term shaping of this UNESCO World Heritage Site in the category of cultural landscape. The study area is situated on a glacial modelled high mountain environment ranging from 1250 to 2800 m.a.s.l. Multidisciplinary approaches integrating archaeology and palaeoenvironment have been directed towards the unravelling of the long-term human–landscape relationships, which ultimately resulted in the MPCV cultural landscape. The development of high-resolution temporal and spatial studies could successfully correlate archaeological and palaeoenvironmental data. This study leads to the location of more than 400 archaeological structures, 55 of which were excavated, and the multiproxy study of 7 palaeoenvironmental sequences. The combination and analysis of all these data have permitted developing a history of human–environment interactions from the Mesolithic to the 20th century. In this paper, data gathered in the MPCV corresponding to the Neolithic and Chalcolithic periods are presented for the first time. During the Early Neolithic small groups are documented with a diversified economy in which grazing, hunting, fishing, gathering and an incipient cereal agriculture activities are well represented. These groups seem to follow highly mobile occupation patterns with continuous high mountain seasonal grazing exploitations that lasted one or two centuries. They appear to frequent diverse altitudinal belts in order to take advantage of different resources. A strong pastoral orientation is related to the exploitation of high mountain areas. During the Middle/late Neolithic human groups show a higher degree of sedentism. Hunting and gathering are still important activities although agriculture and animal husbandry increase in importance. During this period an augmentation in the pastoral pressure in the MPCV is also documented, linked to the first use of fires to create grazing areas. Symbolic landscape appropriation practices are also firstly documented during this period. During the Chalcolithic, human landscape use becomes intensive enough to cause permanent landscape changes. The upper parts of the MPCV are deforested by the action of fire while intensive agriculture takes place at the lower valleys. The evidence presented by the MPCV project demonstrates that it was during the Neolithic when this high mountain cultural landscape was firstly formed. This process is probably related to an increase in the population and progressive sedentism, which required a more intensive and organised use of resources and, eventually, the adoption of landscape management practices.