Green microalgae are widely used for wastewater treatment, food/feed and pigment production, as well as for aquaculture. However, very little is known about their surface composition, which can determine algae behavior in nature and influence their processing. In this work, we use cryo-XPS to characterize the surface chemical composition of three different microalgae species. We investigate the applicability of a data treatment method, developed for bacteria, deconvoluting C 1s with respect to protein, lipid and polysaccharide. We discuss how substances unique to algae contribute to the C 1s spectra and how this affects the transferability of the method to microalgae. Two species of green microalgae isolated from Northern Sweden, Chlorella vulgaris 13-1 and Coelastrella sp. 3-4, were compared to reference culture collection strain, Scenedesmus obliquus RISE (UTEX 417). Cryo-XPS data indicate that surfaces of Coelastrella sp. 3-4 and C. vulgaris 13-1 cells are dominated by protein and carbohydrates. However, the carbohydrate content was higher for C. vulgaris. The reference strain shows the highest content of proteins and has an increased amount of lipids compared to the other two. Estimation of the cell surface hydrophobicity suggests that the hydrophobicity increases in the order: C. vulgaris < Coelastrella sp. < S. obliquus.