Structured liquids,g enerated by the interfacial formation, assembly,a nd jamming of nanoparticle (NP)surfactants at liquid/liquid interfaces,maintain all the desirable characteristics of each liquid, while providing as patially structured framework. Herein, we show that rod-like cellulose nanocrystal (CNC)-based NP-surfactants,t ermed CNC-surfactants,a re formed rapidly at the liquid/liquid interface, assemble into amonolayer,and, when jammed, offer arobust assembly with exceptional mechanical properties.P lateau-Rayleigh (PR) instabilities of af ree-falling jet of an aqueous medium containing the CNCs into atoluene solution of amine end-functionalized polystyrene are completely suppressed, allowing the jetting of aqueous tubules that are stabilized when the CNC-surfactants are jammed at the interface.T hese results open an ew platform for the additive manufacturing techniques,f or example,t hree-dimensional (3D) printing,o f all-liquid constructs.