Research into two-dimensional (2D) materials (analogues of graphene) spans physics, chemistry, and materials science. Accordingly, quantum-mechanical modelling of 2D materials can use approaches and questions that come from physics as well as from chemistry. In this presentation, I will present some examples from our recent work in this area, including: (i) transition metal dichalogenide heterostructures, (ii) interactions of 2D materials with actinides, (iii) interface between 2D material and conducting polymers. I will focus on the kinds of questions that can be addressed, the choices one have to be made in terms of methodology and models, the challenges that arise in this process, and the unique contributions that computational chemistry can make in this area.