The group, which has 15 branches in Scotland and employs more than 50 people here, threw in the towel after lenders said they did not consider options to save the business "capable of being completed".
The appointment of PwC as administrators came as the Reading-based Albemarle admitted that, with no financial support from lenders and mounting trading losses, it would not be seeking an extension to a March 31 restructuring deadline set by its banks.
Trading in the Aim-listed stock was suspended on Monday after lenders, Barclays and Lloyds, rejected plans to save the business.
It abandoned an attempt to sell itself in January, saying none of the proposals represented a fair value for the business.
Plunging gold prices and increased competition left the group struggling with losses and overstretched finances.
Its shares, which were suspended at 6.65p, have lost around 97% of their value in the last year as its woes deepened and investors were warned on Monday that any remaining options for the group would likely wipe out any remaining value of the stock.
Yesterday Albemarle said: "In the absence of any other available facilities from its lenders or elsewhere, the company will shortly be unable to meet its liabilities as they fall due. The board has therefore concluded that, in such circumstances, the appointment of an administrator is the most appropriate course of action."
Albemarle, which has more than 180 outlets, had attempted to turn itself around by slashing costs. It closed 40 pop-up gold stores last year.
It had been given a reprieve by lenders, with a deadline extended further at the beginning of the year, but was unable to come up with a viable rescue solution.
The group has warned that earnings will be significantly below expectations and admitted it had resorted to melting down gold jewellery stocks to raise cash.
There has also been a mass exodus of its board of directors, with five of its six non-executives quitting at the start of December.
The company was founded in Bristol in 1983 with a single shop.
PwC warned some redundancies may be necessary as it confirmed its appointment, although it stressed all staff were being paid as normal in March, including accrued bonuses.
It will seek to sell all or part of the business and said it aimed to "protect as many jobs as possible".
All stores will remain open while it seeks a buyer and landlords have been paid.
PwC said: "Our priority is to keep all pledged items safe and available for redemption as normal."