The search for a geometrical understanding of dualities in string theory, in particular T-duality, has led to the development of modern T-duality covariant frameworks such as Double Field Theory, whose mathematical structure can be understood in terms of generalized geometry and, more recently, para-Hermitian geometry. In this work we apply techniques associated to this doubled geometry to four-dimensional manifolds, and we show that they are particularly well-suited to the analysis of integrability in special spacetimes, especially in connection with Penrose's twistor theory and its applications to general relativity. This shows a close relationship between some of the geometrical structures in the para-Hermitian approach to double field theory and those in algebraically special solutions to the Einstein equations. Particular results include the classification of four-dimensional, possibly complex-valued, (para-)Hermitian structures in different signatures, the Lie and Courant algebroid structures of special spacetimes, and the analysis of deformations of (para-)complex structures. We also discuss a notion of “weighted algebroids” in relation to a natural gauge freedom in the framework. Finally, we analyze the connection with two- and three-dimensional (real and complex) twistor spaces, and how the former can be understood in terms of the latter, in particular in terms of twistor families.