Inspired by previous observations made using Alq3, investigations into the effectiveness of luminophores based on main group metal complexes remain ongoing. Aluminium, due to its ubiquity and nontoxicity, in combination with a suitable ligand, seems to be the ideal candidate for a high-performance luminophore. As evidence, a recently published dimethylaluminium β-oxo-δ-diimine derivative achieves the PLQY of 1 in a toluene solution. However, in the solid its efficiency dropped significantly as a consequence of ACQ. We have now presented a series of novel aluminium-stereogenic anthranilates obtained by a simple synthetic procedure using commercially available anthranilic acid and its derivatives. Strikingly, in the solid state, compound 4, incorporating an anthranilate ligand with a-N bonded phenyl ring, returns a PLQY of 1. To our knowledge, this is the best result to date among Al-based luminophores in the solid state. Overall, the reported results indicate that the observed photophysical processes likely arise from ligand-centred transitions that are facilitated by coordination of the anthranilate ligand to the aluminium centre. Additionally, a particular role for the photophysical performance in the solid state is played by noncovalent interactions that are able to preserve the geometry deformation displayed after excitation and significantly inhibit luminescence-unfavourable relaxation processes. The simplicity of the ligand framework modification offers the possibility of further upgrading of the system to achieve greater chemical stability and enables modulation of the optical properties, which will be important from the point of view of applications.