Witten's higest achievements are based on topological reasoning on low dimensions (up to 4 dimensions). So, you will always see him talking about chern simons theory, mostly in 3d, N=2 supersymmetric models in 4d (e.g. Seiberg-Witten duality), topological strings which are complex 3D, twistors strings lives in 3D complex space CP(3|R).
This is a very convenient way to analyze String Theory because, for example, Calabi Yau manifolds ( the 6 other non "usual" dimensions), which are used to build particles and forces at low energy limits, can be identified with several of the above 3d complex (6d real, roughly) models.
The case of Langlands on Witten's work, at least the impression I have, is trying to study a generalization, or mix, of t'Hooft and Wilson loops. Given that t'Hooft op works as dual (it encloses) to a Wilson loop, which is the path integral of a gauge field, but creates Dirac-string like singularities, you need to study how this singularities interact with such generalization. These singularities correspond to operators on the surface of the enclosing, so studying these operators is like studying the mix of these operators.
These operators correspond to the study of cusps (Langlands), but also to the geometry of the generalization. These generalized space is in 4D, and has elements of 3d and 2d. So, it is a way to work out how different mathematical entities that makes up the above topological theories relate to each other.