The film was shot primarily in two locations: On the edge of Dartmoor, Devon and the area surrounding Dymchurch, Kent. Dymchurch is the setting for the Russell Thorndike novels about 'Doctor Syn' : a pastor / smuggler who disguises himself as a scarecrow to deceive and intimidate his prey.
The lead redcoat looks a lot like Christopher Lee. The reason for this was the costume was on a short term loan and thus one actor had to act all the redcoat roles with the characters faces being illustrated later.
In the final 'epilogue' sequence where the Scayrecrow visits the ghost of Eleanor, when she opens the tavern window, the skull used in the subsequent animation 'The Screaming skull' is seen screen left.
At the end fade out of the Tavern sequence, a folk song can be heard. This song is a traditional one based around the tale of the Lambton worm, which at the time of 'Scayrecrow's production was slated as the next film to be made.
Though seen only fleetingly, the name on the Tavern sign wherein Eleanor Tawney works (Sue Tilbrook) is called 'The Slaughtered Lamb' - which as any horror fan will tell you is a reference to An American Werewolf in London (1981).