Decreasing
the interconnecting temperature is essential for 3D
and heterogeneous device integrations, which play indispensable roles
in the coming era of “more than Moore”. Although nanomaterials
exhibit a decreased onset temperature for interconnecting, such an
effect is always deeply impaired because of organic additives in practical
integrations. Meanwhile, current organic-free integration strategies
suffer from roughness and contaminants at the bonding interface. Herein,
a novel bilayer nanoarchitecture simultaneously overcomes the drawbacks
of organics and is highly tolerant to interfacial morphology, which
exhibits universal applicability for device-level integrations at
even room temperature, with the overall performance outperforming
most counterparts reported. This nanoarchitecture features a loose
nanoparticle layer with unprecedented deformability for interfacial
gap-filling, and a compact one providing firm bonding with the component
surface. The two distinct nanoparticle layers cooperatively enhance
the interconnecting performance by 73–357%. Apart from the
absence of organics, the internal abundant lattice disorders profoundly
accelerate the interconnecting process, which is supported by experiments
and molecular dynamics simulation. This nanoarchitecture is successfully
demonstrated in diversified applications including paper-based light-emitting
diodes, Cu–Cu micro-bonding, and SiC power modules. The strategy
proposed here can open a new paradigm for device integrations and
provide a fresh understanding on interconnecting mechanisms.