A new methodology is developed for local entropy generation analysis of turbulent flows using large eddy simulation (LES). The entropy transport equation is considered in LES and is solved along with continuity, momentum, and scalar transport equations. The filtered entropy equation includes several unclosed source terms that contribute to entropy generation. The closure is based on the filtered density function (FDF) methodology, extended to include the transport of entropy. An exact transport equation is derived for the FDF. The unclosed terms in this equation are modeled by considering a system of stochastic differential equations (SDEs). The methodology is employed for LES of a turbulent shear layer involving transport of passive chemical species, energy, and entropy. The local entropy generation effects are obtained from the FDF and are analyzed. It is shown that the dominant contribution to entropy generation in this flow is due to combined effects of energy transfer by heat and mass diffusion. The FDF results are assessed by comparing with those obtained by direct numerical simulation (DNS) of the same layer. The FDF predictions show favorable agreements with the DNS data.