Surface Segregated AgAu Tadpole‐Shaped Nanoparticles Synthesized Via a Single Step Combined Galvanic and Citrate Reduction Reaction

New AgAu tadpole nanocrystals were synthesized in a one‐step reaction involving simultaneous galvanic replacement between Ag nanospheres and AuCl4−(aq.) and AuCl4−(aq.) reduction to Au in the presence of citrate. The AgAu tadpoles display nodular polycrystalline hollow heads, while their undulating tails are single crystals. The unusual morphology suggests an oriented attachment growth mechanism. Remarkably, a 1 nm thick Ag layer was found to segregate so as to cover the entire surface of the tadpoles. By varying the nature of the seeds (Au NPs), double‐headed Au tadpoles could also be obtained. The effect of a number of reaction parameters on product morphology were explored, leading to new insights into the growth mechanisms and surface segregation behavior involved in the synthesis of bimetallic and anisotropic nanomaterials. Creature feature: New AgAu tadpoles displaying nodular polycrystalline hollow heads and single‐crystalline undulating tails were obtained by a combination of galvanic replacement and precursor reduction (see figure). The results indicated an oriented attachment growth mechanism. Remarkably, a 1 nm thick Ag layer is found to segregate so as to cover the entire surface of the tadpoles.