Modern materials science has witnessed the era of advanced fabrication methods to engineer functionality from the nano- to macroscales. Versatile fabrication and additive manufacturing methods are developed, but the ability to design a material for a given application is still limited. Here, a novel strategy that enables target-oriented manufacturing of ultra-lightweight aerogels with on-demand characteristics is introduced. The process relies on controllable liquid templating through interfacial complexation to generate tunable, stimuli-responsive 3D-structured (multiphase) filamentous liquid templates. The methodology involves nanoscale chemistry and microscale assembly of nanoparticles (NPs) at liquid-liquid interfaces to produce hierarchical macroscopic aerogels featuring multiscale porosity, ultralow density (3.05-3.41 mg cm^-3 ), and high compressibility (90%) combined with elastic resilience and instant shape recovery. The challenges are overcome facing ultra-lightweight aerogels, including poor mechanical integrity and the inability to form predefined 3D constructs with on-demand functionality, for a multitude of applications. The controllable nature of the coined methodology enables tunable electromagnetic interference shielding with high specific shielding effectiveness (39 893 dB cm² g^-1 ), and one of the highest-ever reported oil-absorption capacities (487 times the initial weight of aerogel for chloroform), to be obtained. These properties originate from the engineerable nature of liquid templating, pushing the boundaries of lightweight materials to systematic function design and applications.

Janus structures have unique properties due to their distinct functionalities on opposing faces, but have yet to be realized with flowing liquids. We demonstrate such Janus liquids with a customizable distribution of nanoparticles (NPs) throughout their structures by joining two aqueous streams of NP dispersions in an apolar liquid. Using this anisotropic integration platform, different magnetic, conductive, or non-responsive NPs can be spatially confined to opposite sides of the original interface using magnetic graphene oxide (mGO)/GO, Ti₃C₂T_x/GO, or GO suspensions. The resultant Janus liquids can be used as templates for versatile, responsive, and mechanically robust aerogels suitable for piezoresistive sensing, human motion monitoring, and electromagnetic interference (EMI) shielding with a tuned absorption mechanism. The EMI shields outperform their current counterparts in terms of wave absorption, i.e., SE_T ≈ 51 dB, SE_R ≈ 0.4 dB, and A = 0.91, due to their high porosity ranging from micro- to macro-scales along with non-interfering magnetic and conductive networks imparted by the Janus architecture.