Silicon
is one of the most promising alternative active materials
for next-generation lithium-ion battery (LIB) applications due to
its advantage of high specific capacity. However, the enormous volume
variations during lithiation/delithiation still remain to be an obstacle
to commercialization. In this work, binder-free pure silicon and silicon/carbon
(Si/C) multilayer thin-film electrodes, prepared by scalable one-step
magnetron sputtering, are systematically investigated by an interlayer
strategy. Herein, we present a rationally structural modification
by an amorphous carbon film to enhance the electrical conductivity,
mechanical integrity, and electrochemical performance of Si film-based
LIBs. Therefore, to maintain the consistency of the direct-contact
layer with the electrolyte and current collection, symmetrical Si/C/Si
and Si/C/Si/C/Si/C/Si electrodes are deliberately designed to study
the influence of embedded carbon. An anode with a carbon content of
10.38 wt % yields an initial discharge specific capacity of 1888.74
mAh g–1 and a capacity retention of 96.82% (1243.56
mAh g–1) after 150 cycles at a high current density
of 4000 mA g–1. It also shows that the best rate
capability remains 96.0% of the initial capacity in the 70th cycle.
At last, three mechanisms are proposed for an in-depth understanding
of the interface effect. This work offers a new perspective scheme
toward Si/C-based LIBs with a capability of high rate and high energy
density.