Aluminium borophosphate gels and glasses with different compositions are prepared, for the first time, via the sol–gel process using aluminium lactate, boric acid and phosphoric acid as precursors. This glass-forming range is significantly wider than that accessible via the melt cooling route. The route from the solution to the gel and the final glass is monitored ex-situ by multinuclear high-resolution liquid and solid state NMR techniques, characterizing the influence of composition and temperature on the hydrolysis, polymerization, and vitrification processes. Addition of Al(lact)₃ to H₃BO₃ aqueous solution results in the formation of [B(lact)₂]⁻ species. In the dried xerogels, the boron structure is dominated by the three tetrahedrally coordinated environments involving variable lactate, phosphate and water ligands—[B(lact)₂]⁻, [B(lact)(OH)_2−x(PO₃)_x]⁻, and [B(lact)(OH)_4−x(PO₃)_x]⁻—the fractional concentrations of which are significantly dependent on the gel-forming conditions (e.g. gel-processing temperature and Al/B/P molar ratio). ²⁷Al–¹¹B double resonance experiments suggest that B–O–Al connectivities are not present. The dominant aluminium species present in the xerogel are [Al(lact)₃], [Al(lact)₂(PO₃)₂]⁻, [Al(lact)₁(PO₃)₄]²⁻, and [Al(PO₃)₆]³⁻, involved in various degrees of polymerization. Following the heat treatment of the gel towards glass, the lactate ligands (linked to both B and Al units) are successively replaced by phosphorus ligands, resulting in further structural polymerization. Upon heating to 500 °C, the gels are finally converted to bulk glasses with thermal and structural characteristics close to those of glasses accessible via traditional melt cooling from 1550 °C. Single resonance and ¹¹B{³¹P} and ²⁷Al{³¹P} double resonance NMR results indicate that the extent of B/P and Al/P connectivity in the glasses is generally maximized.