propyl-methacrylate] P(METACco -MPTS) were fi rst attached to the surface of PU sponges by hydrolysis via a grafting onto method, followed by catalyst loading via ion exchange process and metal plating by electroless metal deposition (ELD) process, forming 3D-internected conductive networks of metals. Despite the fruitful realization of highly conductive 3D composites, precisely controlling the molar ratio between METAC and MPTS as well as the viscosity of the polymer solutions are required. Besides that, since a hydrolysis step is involved, a dry storage of polymers as well as the preparation of their solutions in dry condition are needed. In addition, the metal-PU sponges are required to be packaged by infusing with viscous PDMS pre-polymers in order to obtain good performances of stretchability and compressibility. Therefore, it is still highly desirable to develop more convenient methods to fabricate 3D conductive composite materials.To address this need, herein, we report a low-cost, solutionprocessed, versatile approach to fabricate 3D fl exile conductors from PDMS sponges by a combination of surface modifi cation with poly[2-(methacryloyloxy)ethyl-trimethylammoniumchloride] (PMETAC) polymers and consequent electroless metal deposition. Notably, PDMS sponges are one particular type of 3D-interconnected porous structures, which are made of elastomeric materials. Hence, not only the material itself can be stretched, but also the sponge-like structures are highly stretchable. Therefore, PDMS sponges are one type of materials and structures that are particularly suitable for the fabrication of electrically conductive 3D stretchable and compressible electrodes or interconnects. In the present study, pieces of PDMS sponges prepared by using a conventional sugar-templating method were fi rst functionalized with vinyltrimethoxysilane (VTMS) by a silanization process, followed by a typical in situ free radical polymerization step with METAC. The as-made PMETAC-PDMS sponges were then used as 3D-interconnected porous structures for solution-processed electroless metal deposition, leading to the formation of metal-coated PDMS sponges. To validate this method, we have successfully fabricated Cu-, Ag/Cu-, and Au/Cu-PDMS sponges as well as the fl exible circuits to light up light-emitting diode (LED) arrays with good electric conductivity and mechanical stability, such as stretchability and compressibility. Our results show that the resistance of the as-fabricated composite almost maintains a constant under a large number of cycles (up to 5000) of repeated stretching and compressing deformation. The key novelty of this method is that thin layers of metal structures are directly fabricated on a fl exible sponge structures made of elastic PDMS materials. Therefore, the metal-PDMS sponge conductors are highly fl exible in 3D. What is more, compared with our previous studies Flexible electronics, a disruptive technology that is emerging toward a wide variety of new applications, such as wearable electronics, fl exible display...