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Albumin nanocolloids have been used as radiopharmaceuticals for more than 40 years. Their main use is in lymphoscintigraphy and the detection of the sentinel lymph node as part of the surgical treatment of a variety of solid tumours. The main licensed products are labelled with the gamma emitter technetium-99m. Recently, two analogues labelled with positron emitters have been reported, using gallium-68 and zirconium-89. For about 10 years, there has been interest in dual-modal agents with both radioactive and fluorescent labels to improve the localisation of the sentinel lymph node. Indocyanine green (ICG) has been the most widely used fluorescent label, largely due to its availability as a licensed agent and its ease of application. The further development of alternative radiolabels or improved fluorescent tags will require investment in the development and licensing. There is also a vast potential for the targeting of albumin nanocolloids using existing strategies, which could be promising for the development of both diagnostic and therapeutic agents.