There are vague stories, likely based on some fact, of the cave being a smugglers' hideaway and linked with tales of the supernatural. 

It was formally believed to be the abode of spirits who guarded this entrance to the nether world. The first Lord of Reay (Donald Mackay, Chief of Clan Mackay) met with the Devil on several occasions and was able to get the better of him. The Prince of Darkness was none too pleased about this and followed Donald Mackay to Durness where he sought to waylay him in Smoo Cave. Lord Reay was heading for the cavern just before dawn but had the good fortune to send his dog into the blackness in front of him. When the animal came out howling and hairless the master of Reay realised what lay in store for him. He held back for a moment and in that moment the sun rose. In the light of day, the Devil was powerless and left through the roof of the cave leaving the three holes seen today.  

Source: Alexander Polson's Scottish Witchcraft Lore (W. Alexander: Inverness 1932).

Among the many local legends surrounding the cave is that of the feared highway man McMurdo. Legend has it that during the sixteen century, McMurdo murdered his victims by throwing them down the blowhole into the cave. You can still see McMurdo’s tomb at Balnakeil Church which overlooks nearby Balnakeil Bay.  

In or about the year 1720, the Clan Gunn from the borders' of Sutherland made an unexpected raid on the district of Durness. The inhabitants were taken unawares, and being unprepared had no alternative but to resort to stratagem, pretending to flee to safety they enticed the guns to follow them into the depths of the Smoo cave when once there they concealed themselves in the hidden recesses and crevices of this underground passageway in the limestone rocks from which they slaughtered the Gunns to the very last man,

A few years after the 45 rebellion an Inland Revenue Supervisor in the company of another Excise Officer, were ordered by the Government, to suppress the illegal practice of working small stills in the district of Durness, having authority to arrest the person involved in such illicit practices with power to confiscate their distilling plant. The gaugers bribed one, Donald Mackay by name, who resided in the vicinity of the Smoo Cave, to conduct them in his small boat into the inner chambers of the cave, where the illicit practice of distilling was, they had heard, being carried out in regular and uninterrupted fashion.

On this particular occasion on which Donald Mackay was employed by them, the Smoo Burn was in high flood, and on pushing off from the anchorage inside the second chamber of the cave, Mackay observed that the two gaugcrs were literally terrified, as he rowed them into the spray of the waterfall inside it.

Donald Mackay, being a strong swimmer, purposely maneuvered his craft into dangerous proximity to the crashing furies at the base of the fall and purposely capsized the boat, when he swam to safety, leaving the two unfortunate Inland Revenue officers to drown amid the angry, troubled waters. Rumours has it that one of the bodies has never been found to this day; but the ghost of this lost man appears in the foam below the waterfall inside the second chamber of Smoo Cave when the burn is in high flood.

Shortly after this " accident " the distilling plant was tactfully removed to a place of safety and the cave was deserted by the smugglers.

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