Magnetic resonance imaging (MRI) is one key expertise in trendy diagnostic medication. Nonetheless, the event of high-relaxivity distinction brokers with beneficial properties for imaging purposes stays a difficult job. On this work, twin gadolinium(III) and copper(II) doped-layered double hydroxide (GdCu-LDH) nanoparticles present considerably larger longitudinal relaxivity in contrast with sole-metal-based LDH (Gd-LDH and Cu-LDH) nanoparticles. This rest enhancement in GdCu-LDH can also be a lot larger than the straightforward addition of the relaxivity fee of the 2 paramagnetic ions in Gd-LDH and Cu-LDH, presumably attributed to synergistic T1 shortening between adjoining Gd(III) and Cu(II) within the LDH host layers (adjoining impact). Furthermore, our GdCu-LDH nanoparticles exhibit a pH-ultrasensitive property in MRI efficiency and present a lot clearer MR imaging for tumour tissues in mice than Gd-LDH and Cu-LDH on the equal doses. Thus, this novel Gd/Cu-co-doped LDH nanoparticles present larger potential for correct most cancers analysis in clinic software. To the most effective of our data, that is the primary report that two paramagnetic steel ions in a single nanoparticle synergistically enhance the T1-MRI distinction.