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We examine, herein, specific dynamic responses of collagen molecules (i.e., observations of self-assembly and nanometric adhesion force measurements of type-I collagen molecules) as they interact with either a hydrophobic or a hydrophilic surface at two distinct temperatures, using a liquid-type atomic force microscope. We conclude that, regardless of surface hydrophobicity/hydrophilicity, assembled microfibrils eventually distribute homogeneously in accordance with changes in surface-related mechanical properties of collagen molecules at different self-assembly stages.