Abstract Pressure can alter interatomic distances and its electrostatic interactions, exerting a profound modifying effect on electron orbitals and bonding patterns. Conventional pressure engineering relies on compressions from external sources, which raises significant challenge in precisely applying pressure on individual molecules and also consume substantial mechanical energy. Here we report ultrasmall single-layered NbSe 2 flat tubes (< 2.31 nm) created by self-pressurization during the deselenization of NbSe 3 within carbon nanotubes (CNTs). As the internal force (4–17 GPa) is three orders of magnitude larger than the shear strength between CNTs, the flat tube is locked to prevent slippage. Electrical transport measurements indicate that the large pressure within CNTs induces enhanced intermolecular electron correlations. The strictly one-dimensional NbSe 2 flat tubes harboring the Luttinger liquid (LL) state, showing a higher tunneling exponent $${\alpha }_{{NbS}{e}_{2}{{{{{\rm{@}}}}}}{CNT}}\approx 0.32$$ αNbSe2@CNT≈0.32 than pure CNTs ( $${\alpha }_{{CNT}}\approx 0.22$$ αCNT≈0.22 ). This work suggests a novel chemical approach to self-pressurization for generating new material configurations and modulating electron interactions.