electron transport properties and direct band gap structure, InN is a promising candidate for high-speed optoelectronic devices, broad-spectrum solar cells, high electron mobility transistors, near infrared light emitting diodes (LEDs) and high-speed laser diodes [2][3][4]. Furthermore, its nontoxic nature and infrared emission properties enable InN to be used in biological and medical applications [5]. Besides these advantageous properties of InN material, its nanostructures have been widely studied due to their different characteristics depending on the dimensionality and size, which allow the applications in nanoscale electronic and optoelectronic devices [6,7].InN crystallizes in two different structures: stable hexagonal (wurtzite) structure and metastable cubic structure. When compared to hexagonal InN, cubic InN possesses smaller band gap and superior electronic properties due to its isotropic lattice and lower phonon scattering [8]. However, the production of cubic InN-NCs is quite a challenging process due to its thermodynamically unstable nature [9]. Previous studies showed a number of techniques viable for the synthesis of InN-NCs mainly having hexagonal structure. Ambient pressure and low-temperature liquid phase was proposed as a suitable method for the synthesis of nanoparticles having low decomposition temperatures. It was shown that wurtzite InN-NCs having 6.2 nm average diameter are successfully produced using this method. These colloidal wurtzite InN-NCs were post-treated with nitric acid to get rid of the metallic indium byproduct and finally InN nano-powder was obtained [10]. Moreover, activated reactive evaporation and nitrogen plasma annealing methods were proposed for the successful production of wurtzite InN-NCs and InN nanorods, respectively. It was suggested that the technique is applicable to produce InN-NCs by using low temperatures from indium nanostructures obtained by different techniques [11]. Xiao et al.Abstract Nanostructures of InN have been extensively investigated since nano-size provides a number of advantages allowing applications in nanoscale electronic and optoelectronic devices. It is quite important to obtain pure InN nanocrystals (InN-NCs) to reveal the characteristic features, which gain interest in the literature. Here, we proposed a new approach for the synthesis of ultra-small hexagonal InN-NCs by using suspension of micron-sized InN powder in ethanol with pulsed laser ablation method. The liquid environment, laser energy and ablation time were optimized and a post-synthesis treatment, centrifugation, was performed to achieve InN-NCs with the smallest size. Besides, the micron-sized InN powder suspension, as a starting material, enabled us to obtain InN-NCs having diameters smaller than 5 nm. We also presented a detailed characterization of InN-NCs and demonstrated that the formation mechanism mainly depends on the fragmentation due to laser irradiation of the suspension.