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It is likely that metal mining had been undertaken at Llangynog since prehistoric or Roman times, but the first major discovery of lead ore came in 1692.
In the early 18th century the Llangynog lead mines were among the richest in Britain. Most of the shafts were sunk on the slopes of Cyrniau, south of the village, with galleries extending under the valley floor, but there were other mines on Craig Rhiwarth and in Cwm Orog. Spoil heaps are visible on Cyrniau and in the area now used by the Revolution Bike Park: the chimney of a smelter has survived further up the lane that leads there. Lead mining ceased in 1916.
Slate quarrying was also a major industry, and was certainly under way by 1705. Llangynog slates were well known for their quality and durability. The largest quarry (in fact an underground mine) was to the north of the village on the slopes of Craig Rhiwarth, where the line of the main incline is visible from the car park among large areas of slate waste: other quarries can be seen above the village on the ridge known as Y Gribin and up the Pennant road. Slate production ceased during the Second World War.
Granite quarrying was also important during the first half of the 20th Century. Today the scars are healing, and employment locally is restricted to agriculture and small scale craft or leisure enterprises.