We have synthesized flexible monolithic carbon aerogels by incorporating diatomite as antishrinkage agent during the sol-gel polycondensation of the precursors. The materials displayed elastic properties and preserved their pristine dimensions upon densification by carbonization even after etching of the diatomite, due to the open pore structure of the siliceous additive in the material's matrix. The aerogels displayed a well-developed porous structure, confirming that the polymerization of the precursors is not impeded; the effect of the additive was independent of the formulation of the aerogels, as evidenced by the behavior of aerogels with varied composition (molar ratio, pH, N-doping).After the early works of Pekala and coworkers on the synthesis of carbon aerogels by the solgel polycondensation of resorcinol (R) and formaldehyde (F) mixtures [1,2], the interest for these solids has raised due to their potential use in several fields. Despite their versatility, the technological applications of carbon aerogels have often been limited by their poor mechanical properties. The mechanical stiffness of carbon aerogels depends strongly on the 2 porosity and the degree of cross-linking of the precursors [2,3]. The usually fragile hydrogels are mechanically reinforced upon carbonization as they become more rigid with increased Young modules [2,3], but their deformation capacity decreases. In previous works we have reported the preparation of carbon aerogels using various precursors with enhanced conductivity and chemical resiliency to oxidation [4,5]. Despite the good electrochemical performance, the use of monolithic electrodes was limited due to the large shrinkage and deformation of the pieces after carbonization -leading to densification of the matrix-[5]; this is a challenge for electrochemical applications where the contact between the electrode material and the current collector is crucial to avoid efficiency losses due to resistance.Aiming at fabricating large monolithic electrodes with improved mechanical properties without adversely affecting their porosity and conductivity, we herein report the preparation of monolithic carbon aerogels with enhanced mechanical properties by using a low cost siliceous sacrificial additive (i.e. diatomite earth). The synthesis route is a simple modification of the conventional one reported elsewhere [4], and consists on allowing the sol-gel polymerization of the precursors in the presence of the additives; after the supercritical drying step, the hydrogels (series H-) were carbonized (series C-), and the siliceous additive was finally removed by HF etching (see further details in the ESI File). Selected formulations with different precursor's molar ratio (R, F and melamine, M) and additives (either diatomite (D), carbon black (B), or both) were prepared (Table 1), to show that the effect of the additive does not depend on the composition of the aerogels. From a macroscopic point of view ( Fig. 1), the materials ranged from translucent (pristine) to opaque when eith...