This paper presents the development of novel Carbon-Fibre Reinforced Polymer (CFRP) laminates, tailored for the application of Digital Volume Correlation (DVC) and Computed Tomography (CT) to experimental mechanics analyses of these materials. Analogous to surface-based Digital Image Correlation (DIC), DVC is a relatively novel volumetric method that utilizes CT data to quantify internal three-dimensional (3D) displacements and implicit strain fields. The highly anisotropic and somewhat regular/self-similar microstructures found in well-aligned unidirectional (UD) materials at high fibre volume fractions are intrinsically challenging for DVC, especially along the fibre direction at microstructural length-scales on the order of a few fibre diameters. To permit the application of DVC to displacement and/or strain measurements parallel to the fibre orientation, the matrix was doped with a sparse population of sub-micrometre particles to act as displacement trackers (i.e. fiducial markers). Barium titanate particles (400 nm, ∼1.44 vol. %) were found to offer the most favourable compromise between contrast in CT images and the ability to obtain a homogeneous distribution in 3D space with sufficient particle compactness for local DVC analyses. This property combination was selected following an extensive Micro-focus Computed Tomography (µCT)-based qualitative assessment on a wide test matrix, that included 38 materials manufactured with a range of possible particle compositions, mean sizes and concentrations. By comparing the tensile behaviour of the particle-adapted material alongside its particle-free counterpart, we demonstrate through the application of in situ Synchrotron Radiation Computed Tomography (SRCT) that the macro- and micromechanical responses of the newly developed CFRP are consistent with standard production materials indicating its suitability as a model system for mechanistic investigations.