Recently, the potential of electrospun fibers was reported for the fabrication of novel electrospun fibrous sponges by the use of short electrospun fibers. [4,6,14,16] Owing to flexible fabrication conditions and diversified electrospun fibers, the sponges displayed tunable densities, multifunctionality, and applicability for various applications, for instance, reversible manual compression, [16] hydrophilic or super hydrophobic, [17,18] electrics, [19,20] respirable open cells, [21] or scaffolds for tissue engineering. [22,23] Thus, these sponges could perfectly overcome the mechanical brittleness of traditional inorganic aerogel and high cost of carbon aerogel problems, making them a perfect candidate for broad applications due to their high potential for functionalization.So far, almost all the concepts to obtain ultralight sponges consist of fabrication of short electrospun fiber suspensions by mechanical cutting and processing by self-assembly, followed by freeze-drying. [10] Normally, the short fibers obtained by using mechanical cutting devices, such as homogenizer, mixer, blender, grinder, exhibit uncontrollable length and broad length distribution represented by the high coefficient of variation (CV), [3,[24][25][26] which is defined as the ratio of the standard deviation to the mean length. Simultaneously, beyond several different reported methods, such as chemical treatment, [27] ultrasonication, [28] electric spark, [29] concentrated polymer brush, [30] and direct electrospinning, [31][32][33] the patterned UV-crosslinking [34] and microcutting method [35,36] based on highly aligned fibers enable the production of quasi-monodisperse short fibers. Short fiber dispersions with low CV have not been used to the best of our knowledge for the preparation of sponges. Consequently, the role of CV and fiber length in the morphology and mechanical properties of the sponges is unknown, which is, however, very important for basic understanding and numerous applications.Herein, we present a new method for the preparation of short electrospun fiber dispersions with controlled CV and use them for the preparation of the sponges in order to evaluate the microstructure and mechanical properties. We show the cryo-microcutting of multifibrillar highly oriented electrospun poly(acrylonitrile) (PAN) yarns which resulted finally in short individual PAN fibers of well-controlled length. Fiber dispersions of different CVs were obtained by mixing of short fibers of different lengths, which were used for the preparation of sponges following the established method. We could clearly Ultralight highly porous sponges made of short electrospun polymer fibers have gained significant attention for a variety of applications. According to the established procedures, short electrospun fibers are obtained by cutting or homogenization of electrospun fibers in suspension, which yield fibers with inhomogeneous fiber length. The role of the fiber length distribution and the fiber length in the mechanical compressibility of the sponges is unkn...