This paper presents results from an integrated programme of landscape, buildings and materials analysis undertaken at Castle Sween under the aegis of the Scottish Medieval Castles & Chapels C14 Project (SMCCCP). A suite of petrographic, archaeobotanical and radiocarbon analyses are employed to present the first independent dating evidence relating to the construction of three phases of the castle complex, including a primary phase curtain-walled enclosure widely regarded as mainland Scotland’s earliest surviving medieval masonry castle. This data is generally consistent with previous interpretations of the building’s stratigraphy and architectural style, although an earlier than expected determination for the northeast tower draws further attention the contrasting character of this particular structure. Archaeobotanical analysis of the largest assemblage of mortar-entrapped relict limekiln fuel fragments undertaken by the project, thus far, also hints at wider changes in the surrounding environment. Correlating this buildings evidence with palynological and other data associated with the political, vegetational and climate history of the surrounding lordship, and across Argyll more widely, is beginning to align the construction of Castle Sween with broader ecological processes from which the surrounding environment has emerged.