We construct and study a closed, 2-dimensional, quasi-topological (0,2) gauged sigma model with target space a smooth G-manifold, where G is any compact and connected Lie group. When the target space is a flag manifold of simple G, and the gauge group is a Cartan subgroup thereof, the perturbative model describes, purely physically, the recently formulated mathematical theory of "Twisted Chiral Differential Operators". This paves the way, via a generalized T-duality, for a natural physical interpretation of the geometric Langlands correspondence for simply-connected, simple, complex Lie groups. In particular, the Hecke eigensheaves and Hecke operators can be described in terms of the correlation functions of certain operators that underlie the infinite-dimensional chiral algebra of the flag manifold model. Nevertheless, nonperturbative worldsheet twisted-instantons can, in some situations, trivialize the chiral algebra completely. This leads to a spontaneous breaking of supersymmetry whilst implying certain delicate conditions for the existence of Beilinson-Drinfeld D-modules. Via supersymmetric gauged quantum mechanics on loop space, these conditions can be understood to be intimately related to a conjecture by Hohn-Stolz [1] regarding the vanishing of the Witten genus on string manifolds with positive Ricci curvature. An interesting connection to Chern-Simons theory is also uncovered, whence we would be able to (i) relate general knot invariants of three-manifolds and Khovanov homology to "quantum" ramified D-modules and Lagrangian intersection Floer homology; (ii) furnish physical proofs of mathematical conjectures by Seidel-Smith [2] and Gaitsgory [3, 4] which relate knots to symplectic geometry and Langlands duality, respectively.