We propose a simple, low-cost, and large-area method to increase thethermoelectricfigure of merit (ZT) in silicon membranes by the deposition of an ultrathinaluminum layer. Transmission electron microscopy showed that short deposition ofaluminum on a silicon substrate covers the surface with an ultrathin amorphousfilm, which,according to recent theoretical works, efficiently destroys phonon wave packets. As a result,we measured 30?40% lower thermal conductivity in silicon membranes covered withaluminumfilms while the electrical conductivity was not affected. Thus, we have achieved40?45% higher ZT values in membranes covered with aluminumfilms. To demonstrate apractical application, we applied this method to enhance the performance of a silicon membrane-based thermoelectric deviceand measured 42% higher power generation.