Molecularly imprinted nanoparticles were synthesised via iniferter polymerisation in the presence of a chain terminator agent and at high monomer and template concentration. The amount of initiator, chain terminator agent and UV irradiation time were optimised in order to achieve maximum yield of discrete nanoparticles without causing macrogelation of the polymerisation mixture. Resultant particles were then purified from unreacted monomers via gel permeation and characterised by size-exclusion chromatography, dynamic light scattering and electron microscopy. The affinity towards the target was verified via surface plasmon resonance on immobilised templates. The yield of nanoparticles obtained using this approach was 14%, a significant increase when compared with similar methods using high monomer concentration and UV initiation.