We have designed and synthesized over 100 different compounds targeting the blebbistatin site of myosin 2. Based on their inhibitory properties on six myosin-2 isoforms including skeletal, cardiac, smooth and NM2A/B/C, we have made a detailed SAR analysis. We found that the maximal ATPase inhibition can be modulated between 0-100% by the chemical structure of the drug. This unique property of the series of these drugs provides a great pharmacological advantage because the physiological effect can be modulated by the maximal ATPase inhibition and not only by the drug dosage. In order to correlate the compounds’ inhibitory profiles with their effects on cell migration, cell shape formation and neurite outgrowth, the compounds were tested on several human neuronal and fibrocyte cell lines. Besides the general characterization two disease indications are being elaborated. (1) A highly specific drug to skeletal muscle myosin 2 was found to be an efficient muscle relaxant without causing any effect on other physiological processes including heart function and smooth muscle related functions. The specificity relies on a residue that is Leu490 in human skeletal muscle myosin-2s where all the other myosin-2 isoforms have Phe. (2) We developed a compound which can be administered into the ischemic focus of stroke in rat brain and significantly increased ischemic regeneration visualized by MRI, SPECT and PET-CT. The drug treatment drastically improved the general and focal symptoms of stroke compared to the control. These compounds demonstrate that the blebbistatin site of myosin-2 is a pharmacologically highly relevant target.