Optical nanoparticle pH sensors designed for ratiometric measurements have previously been synthesized using post-functionalization approaches to introduce sensor molecules and to modify nanoparticle surface chemistry. This strategy often results in low control of the nanoparticle surface chemistry and is prone to batch-to-batch variations, which is undesirable for succeeding sensor calibrations and cellular measurements. Here we provide a new synthetic approach for preparing nanoparticle pH sensors based on self-organization principles, which in comparison to earlier strategies offers a much higher design flexibility and high control of particle size, morphology and surface chemistry.