Lay out a good looking, clear CV, written on one side of A4 paper.
Include any technical qualifications and exam results, and your basic employment facts and dates. Include voluntary work and anything that shows that you go out and try to make things happen or help people rather than playing computer games in your bedroom, (not saying that you do).
Think about the person reading it and make it easy and quick for them to assimilate and put your CV on the 'Keep' pile rather than into the waste bin.
Advice varies on this, but I included a photo, (of me smiling naturally, wearing a collar and tie and looking pleasant).
Print it on nice watermarked paper.
Post it to every operator you can think of - find out the name of the person responsible for recruitment and address it to them by name. Include a covering letter.
Repeat the above every 2 months or so - the Employer's CV pile will get dumped in the bin every so often, so you need to keep your CV appearing on their desk. But not too often, and don't try to speak to the Chief Pilot in person, they don't appreciate it.
Emails are easily missed amongst an in-box full of several hundred others, but an actual paper envelope and CV on "posh" watermarked paper arriving at the Chief Pilot's desk will, at least be read.
If you hear anything about a company possibly looking for a few pilots. Print out your CV again, put it in an envelope, drive to the head office there and then, and ask reception if they would kindly pass your CV on to the Chief Pilot.
Improve your licence if possible and affordable; e.g. relevant type rating, Instrument rating etc. Back in the day, I spent my last £3,000 on a Shorts 360 type rating, which several UK operators flew at the time.
Good luck
(I did all the above and was eventually successful).