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Sensing self-assembly of polyelectrolyte is critical to exert greater control over layer thickness and properties. The authors demonstrate the use of a scanning probe microscope cantilever-based micromechanical device to sense the self-assembly of polyethyleneimine and polyacrylic acid. A change in mass of the cantilever due to the assembly was recorded by analyzing resonance frequency shift. Experimental results show three orders more sensitive than the conventional quartz crystal sensor. The ratio between the mass of the adsorbed polyelectrolyte and the mass of the polyelectrolyte monolayer is used to evaluate surface coverage as a parameter of critical importance for nanobiotechnology applications.