I've just hired a Junior Designer, whittled down from over a hundred applicants, here's what I'd recommend....

Cover Letter, I know it gets tiring writing multiple cover letters and it's tempting to write a short template and copy/paste, but if you really wanted the job at a company, you'd tell them as much in the cover letter.

Portfolio. Needs to have immediate impact, I looked at each and every portfolio sent to me before any CV, I'd also dismiss people entirely on a poor portfolio without looking at their CV. Experience is irrelevant if you've spent your time well and have a lot to show for it.

Clutter. Be direct, to the point, don't have 'Skill Gauges' on your CV or Portfolio, I don't need to know you've got 1 star of ability in Dreamweaver, I'd prefer to see that you once spent a weekend redesigning the branding for your local bar.

Be Prepared. Sounds obvious, but be yourself in any interview situation, it surprised me how often I was given nervously rehearsed stock interview answers to my questions. Interviews might seem daunting but it's just another conversation with someone you want to be working alongside the following week, have some real questions about the company and the individual, do they have any personal projects?

Know what you want. Sometimes applying for so many jobs becomes a blur, and all you want is just to be employed. You should know the value of good design and expect the person interviewing you to as well. Don't settle for a bone being thrown your way.

Hope this helps.