A full lithium-ion battery cell has been assembled based on nanoarchitectured ternary manganese–nickel–cobalt compounds, in which multi-shell spherical Mn_0.54Ni_0.13Co_0.13(CO₃)_0.8 serves as the anode and the subsequently lithiated Li-excess Li[Li_0.2Mn_0.54Ni_0.13Co_0.13]O₂ with a yolk–shell structure acts as the cathode. The performance of a lithium-ion full battery significantly relies on the electrochemical properties of both anode and cathode materials. A multi-shell carbonate anode is first tested in a half battery cell with metallic lithium as the counter electrode, revealing an unexpectedly high initial charge capacity of 1173.1 mA h g⁻¹ at a specific current of 25 mA g⁻¹, which is two times higher than its theoretical capacity. Moreover, when cycled at 250 mA g⁻¹ for 100 electrochemical cycles, this carbonate anode retains a final specific capacity of 434.6 mA h g⁻¹. Accordingly, a yolk–shell-structured Li-excess layered cathode material has been facilely obtained through lithiation of carbonate compounds, showing an initial discharge capacity of 250.7 mA h g⁻¹ when cycled at 0.1 C (1 C = 250 mA g⁻¹) in a half battery cell. Furthermore, this cathode retains a final capacity of 156.3 mA h g⁻¹ at 1 C after 100 cycles and exhibits an outstanding capacity retention of 90.3%. Such remarkable electrochemical properties of carbonate anode and Li-excess oxide cathode materials are attributed to their nanoarchitectures resulting from the water-based solvothermal process, i.e., multi-shell and yolk–shell structures composed of numerous primary nanoparticles, in comparison with mediocre performances from monodispersive carbonate microspheres and Li-excess oxide nanoparticles synthesized via an ethylene-glycol-based solvothermal method. Combination of the nanostructured ternary transition metal carbonate anode and the Li-excess layered cathode into a full lithium-ion battery results in a remarkable specific capacity above 250 mA h g⁻¹ at 0.1 C in the voltage range of 0.1–4.0 V, which demonstrates the application as a very promising electrochemical device for future energy conversion and storage.