Purpose - Both intravenous thrombolysis (IVT) and intra-arterial endovascular thrombectomy (ET) improve the outcome of patients with acute ischaemic stroke, with ET being an option for those patients with large vessel occlusions. We sought to understand how organisation of services affects time to treatment for both IVT and ET.Method - A multi-objective optimisation approach was used to explore the relationship between the number of IVT and ET centres and times to treatment. The analysis is based on 238,887 emergency stroke admissions in England over three years (2013-2015).Results - Providing hyperacute care only in comprehensive stroke centres (CSC, providing both IVT and ET, and performing >150 ET per year, maximum 40 centres) in England would lead to 15% of patients being more than 45 minutes away from care, and would create centres with up to 4,300 stroke admissions/year. Mixing hyperacute stroke units (HASUs, providing IVT only) with CSCs speeds time to IVT and mitigates admission numbers to CSCs, but at the expense of increasing time to ET. With 24 CSC and all remaining current acute stroke units as HASUs, redirecting patients directly to attend a CSC by accepting a small delay (15-minute maximum) in IVT reduces time to ET: 25% of all patients would be redirected from HASUs to a CSC, with an average delay in IVT of 8 minutes, and an average improvement in time to ET of 80 minutes. The balance of CSC:HASU admissions would change from 24:76 to 49:51.Conclusion - Planning of hyperacute stroke services is best achieved when considering all forms of acute care and ambulance protocol together. Times to treatment need to be considered alongside manageable and sustainable admission numbers.