This paper presents a method of using particle probe scanning force microscopy to measure the adhesion between steel microspheres and cement pastes. Particle probes were fabricated by attaching steel microspheres to the free ends of microcantilevers. Adhesive forces were collected between steel microspheres and new (4-week old) and old (6-month old) cement substrates in air and saturated lime water. For new cement in saturated lime water, adhesive forces between steel and low density C-S-H, high density C-S-H and other hydrated products were intermediate among all groups selected. The adhesive forces between steel and calcium hydroxide were the smallest, whereas the adhesive forces between steel and the unreacted phases were the largest. For the 6-month old cement, the interweaving of calcium carbonate crystals and C-S-H during carbonation generated greater adhesive forces to steel.