It is generally challenging to probe the molecule structure of chlorinated sites in inorganic materials. Energy-filtered microscopy and XPS are commonly used to reveal Cl atoms but provide limited information about the chemical structure. Cl has a nuclear spin of 3/2, a natural isotopic abundance of 75% and a gyromagnetic ratio close to that of N, making it appealing for solid-state NMR experiments. However, acquisition of Cl solid-state NMR spectra is often challenging because quadrupolar signal broadening results in central-transition (CT) NMR spectra that are typically megahertz broad, especially for terminal, covalently bonded Cl atoms. Cl solid-state NMR spectra are generally obtained under static conditions with Car-Purcell-Meiboom-Gill (CPMG) and frequency-stepped acquisition techniques. Unfortunately, static Cl solid-state NMR experiments often suffer from poor sensitivity and resolution. Here, we show 1 H{ 35 Cl} and 29 Si{ 35 Cl} Resonance-Echo Saturation-Pulse DOuble-Resonance (RESPDOR) NMR experiments to directly confirm the presence of chlorinated Si atoms in Si-NS. This approach should be generally applicable to rapidly detect the presence of Cl substituents in inorganic materials at routinely accessible magnetic fields.