With recent advances in nanotechnology, various nanomaterials have been used as drug carriers in molecular imaging for the treatment of cancer. The unique physiochemical properties and biocompatibility of gold nanoparticles have developed a breakthrough in molecular imaging, which allows exploration of gold nanoparticles in drug delivery for diagnostic purpose. The conventional gold nanoparticles synthetisation methods have limitations with chemical contaminations during the synthesisation process and the use of higher energy. Thus, various innovative approaches in gold nanoparticles synthetisation are under development. Recently, studies have been focused on the development of eco-friendly, non-toxic, cost-effective and simple gold nanoparticle synthesisation. The pulsed laser ablation in liquid (PLAL) technique is a versatile synthetic and convincing technique due to its high efficiency, eco-friendly and facile method to produce gold nanoparticle. Therefore, this study aimed to review the eco-friendly gold nanoparticle synthesisation method via the PLAL method and to characterise the gold nanoparticles properties for molecular imaging. This review paper provides new insight to understand the PLAL technique in producing gold nanoparticles and the PLAL parameters that affect gold nanoparticle properties to meet the desired needs in molecular imaging.