A systematic spectroscopic characterization of highly homogeneous water suspensions of ‘buckydiamonds’ comprising sp³ cubic nanodiamond (ND) core covered with disordered sp² shell densely decorated with oxygen-containing groups demonstrates the excitation-wavelength-dependent photoluminescence (PL) given by at least four types of specific structures on the ND surface (hydroxyl, C=O containing ketones, carboxylic anhydrides, and carboxyl groups). PL properties of NDs suspensions possess concentration-dependent behavior revealing tendency of NDs to agglomerate. PL of NDs has been found to be strongly sensitive to pH of the environment in wide range of pH values, i.e. 2–11. We disclosed the mechanisms of pH sensitivity of the ‘buckydiamond’ and proved that it can serve as all-optical sensor of tiny pH variations suitable for further exploitation for pH sensing locally in the area where NDs have been delivered for any purpose, e.g. bioimaging or therapeutic needs.

One-pot hydrothermal synthesis of boron nitride quantum dots (BNQDs) offers a simple and widely accessible approach to produce nanoparticles with tailored properties for biomedical purposes, including bioimaging and drug delivery. However, growing evidence suggests that most reported BNQD syntheses yield products with insufficient purity and poorly defined structures, limiting their bioapplications where precise composition and controlled synthesis are paramount. In this study, we present a formation mechanism and demonstrate multiple BNQD synthesis pathways that can be precisely controlled by modulating the reaction equilibrium during hydrothermal synthesis under varying experimental conditions. We demonstrate that carbon-related defects shift BNQD photoluminescence (PL) from the UV to the 400–450 nm region, making them suitable for bioimaging, while BO₂⁻ enrichment introduces additional phosphorescence. Furthermore, we show that as-synthesized BNQD suspensions contain significant contamination by non-luminescent ammonium polyborate salts, which is overlooked in prior studies, and disclose the mechanism of their formation as well as effective purification method. Finally, we assess the biocompatibility of purified BNQDs with tuned PL properties and demonstrate their application in bioimaging using Vero cells. The elucidated nanoparticle formation mechanisms, combined with methods for precise control of optical properties, structural defects and sample purity, enable the reproducible production of reliable and effective BNQDs for bioimaging.