An ultralight graphene oxide (GO)/polyvinyl alcohol (PVA) aerogel (GPA) is proposed as a new class of acoustic materials with tuneable and broadband sound absorption and sound transmission losses. The interaction between GO sheets and PVA molecules is exploited in our environmentally friendly manufacturing process to fabricate aerogels with hierarchical and tuneable porosity embedded in a honeycomb scaffold. The aerogels possess an enhanced ability to dissipate sound energy, with an extremely low density of 2.10 kg m−3, one of the lowest values ever reported for acoustic materials. We have first experimentally evaluated and optimised the effects of composition and thickness on the acoustic properties, namely sound absorption and sound transmission losses. Subsequently, we have employed a semi-analytical approach to evaluate the effect of different processing times on acoustic properties and assessed the relationships between the acoustic and non-acoustic properties of the materials. Over the 400–2500 Hz range, the reported average sound absorption coefficients are as high as 0.79, while the average sound transmission losses can reach 15.8 dB. We envisage that our subwavelength thin and light aerogel-based materials will possess other functional properties such as fire resistance and EMI shielding, and will prove to be novel acoustic materials for advanced engineering applications.