The poor light absorption of visible light for Cs4PbBr6 nanocrystals (NCs) has severely impeded their practical applications. Although the semiconductor/perovskite heterostructure holds great promise for enhancement in absorption, it has remained a serious challenge for synthesizing a semiconductor/perovskite heterostructure. In this work, monodispersed Janus heterostructures composed of Cs4PbBr6 decorated with either multiple Ag or single Ag on its surface (named as mAg/Cs4PbBr6 and sAg/Cs4PbBr6 respectively), are successfully prepared. The size of Ag seeds has an important effect on the shape of the products. Small-sized Ag seeds lead to the formation of mAg/Cs4PbBr6 Janus NCs, while relatively large-sized Ag seeds produce sAg/Cs4PbBr6 Janus NCs. It is noted that this work not only provides a novel method for the modification of individual Cs4PbBr6 NCs, but also enhances the absorption of the Cs4PbBr6 in the visible region, indicating great potential for optoelectronic applications, such as photocatalysis and solar cells.