We investigated perception of mouthfeel in Pinot noir wines and its physicochemical determinants. Seventeen wine professionals judged 18 Pinot noir wines via two tasting tasks, Descriptive Rating and Directed Sorting, the latter based on perception of in-mouth attributes. Selected chemical measures of the same 18 wines were determined. Sensory results demonstrated that mouthfeel attributes driving high quality were smoothness/silky/velvety, volume/fullness/roundness, overall body, and viscosity/mouth-coating, while the taste of bitterness and perceived tannin harshness drove low quality judgments. Perceived astringency and expressions of tannin (e.g., soft; harsh; fine) drove sorting behaviour of participants. Partial least squares regression (PLSR) was used to associate perceived in-mouth phenomena and chemical composition. The phenolic profile, in particular tannin concentration and structure, was the most important predictor of astringency and its sub-components. These results have important implications for wine producers aiming to enhance perceived quality in their Pinot noir wines.