There is a general separation between the manufacturing processes that add value to materials on the factory floor and the techniques engineers use in the laboratory to evaluate the microstructures and the surface integrity that results. These techniques are often destructive or require a vacuum and are incompatible with production lines. However, this information has intrinsic value and could be exploited to inform production decisions during manufacture. In this study, a novel approach to acquire this information is presented that is underpinned by electrolyte jet machine tool coupled with optical microscopy, which can allow the extraction of both grain-wise partial orientation and morphological information, and crystallographic macro textures in three dimensions. Here, iterative sections are precisely machined into the near surface of a commercially pure titanium alloy using an electrochemical jet and subsequently imaged, allowing the reconstruction of high-fidelity microstructure models rapidly and under ambient conditions. In doing so, new insights into the specific orientation-dependent dissolution mechanisms are offered, and the acquisition of appropriate conditions that result in nanoscale roughness surfaces (avoiding the dominance of pitting and preferential grain removal) is firstly explored. Building on prior work, a piecewise approach is presented to analyse the acquired image stacks to map partial crystal orientations, while different approaches are proposed to account for jet-specific surface artefacts and waviness. This is repeated over 20 layers in an individual specimen and layer-wise orientation maps are used to construct volumetric models of the specimen. These data sets are then explored from the perspective of materials/manufacturing engineers, who may use to this information to effect advancements to materials processing technologies.