The prevalence of microplastics (MPs) in both urban and aquatic ecosystems is concerning, with wastewater treatment plants being considered one of the major sources of the issue. As the focus on developing sustainable solutions increases, unused remnants from bacterial cellulose (BC) membranes were ground to form BC hydrogels as potential bioflocculants of MPs. The influence of operational parameters such as BC:MPs ratio, hydrogel grinding, immersion and mixing time, temperature, pH, ionic strength, and metal cations on MPs flocculation and dispersion were evaluated. A response surface methodology based on experimental data sets was computed to understand how these parameters influence the flocculation process. Further, both the BC hydrogel and the hetero-aggregation of MPs were characterised by UV–Vis, ATR-FTIR, IGC, water uptake assays, fluorescence, and scanning electron microscopy. These highlights that the BC hydrogel would be fully effective at hetero-aggregating MPs in naturally-occurring concentrations, thereby not constituting a limiting performance factor for MPs' optimal flocculation and aggregation. Even considering exceptionally high concentrations of MPs (2 g/L) that far exceed naturally-occurring concentrations, the BC hydrogel was shown to have elevated MPs flocculation activity (reaching 88.6%: 1.77 g/L). The computation of bioflocculation activity showed high reliability in predicting flocculation performance, unveiling that the BC:MPs ratio and grinding times were the most critical variables modulating flocculation rates. Also, short exposure times (5 min) were sufficient to drive robust particle aggregation. The microporous nature of the hydrogel revealed by electron microscopy is the likely driver of strong MPs bioflocculant activity, far outperforming dispersive commercial bioflocculants like xanthan gum and alginate. This pilot study provides convincing evidence that even BC remainings can be used to produce highly potent and circular bioflocculators of MPs, with prospective application in the wastewater treatment industry.