Sensing, localising and identifying individual nuclear spins or frequency components of a signal in the presence of a noisy environments requires the development of robust and selective methods of dynamical decoupling. An important challenge that remains to be addressed in this context are spurious higher order resonances in current dynamical decoupling sequences as they can lead to the misidentification of nuclei or of different frequency components of external signals. Here we overcome this challenge with engineered quantum sensing sequences that achieve both, enhanced robustness and the simultaneous suppression of higher order harmonic resonances. We demonstrate experimentally the principle using a single nitrogen-vacancy center spin sensor which we apply to the unambiguous detection of external protons. Introduction.-The detection of single nuclear spins represents an important yet challenging step towards single molecule magnetic resonance spectroscopy and imaging [1] which holds the promise for the observation of individual protein structures without the need for crystallization of large ensembles. The achievement of this goal may have significant impact on structural biology and medical imaging and may also provide a new tool for the investigation of nuclear spin dynamics in non-trivial quantum biological processes [2,3]. Recently, research has made impressive progress in single nuclear spin detection using various physical platforms [4][5][6][7][8], particularly in the highly challenging task of detecting single spins in external molecules [9][10][11][12][13][14]. Among those physical platforms, a sensor based on individual negatively charged nitrogen-vacancy (NV) centers in diamond [15,16] has demonstrated appealing prospects for applications in biology and medicine, due to its biocompatibility, nano-scale size and long coherence times under ambient conditions [17,18]. NV centers, shallowly implanted to within a few nanometers below the diamond surface, enable strong coupling between NV sensors and target nuclei, thereby promoting the detection sensitivity from a relative large ensemble of nuclei [9,10] to single nuclear spin sensitivity in small clusters of nuclear spins [11][12][13][14]. Besides the interest in single molecule magnetic resonance spectroscopy and imaging, single nuclear spin addressing also has an important role to play in the precise coherent control of nuclear spin qubits, where it may facilitate the realisation of quantum memories with long coherence times and nuclear spin based quantum information processors [19][20][21][22].One ultimate goal of single molecule magnetic resonance spectroscopy using a single spin sensor is to detect a single nuclear spin and further infer the structure of a single molecule