I'll add my two cents.
Yes. Get your CFI. You will improve your knowledge and understanding, improve your communication skills, improve your self-confidence.
There's no down-side.
Then get your CFII, and MEI for the same reasons.
I will be the lone wolf who disagrees that you "need" to go to the regionals to achieve your goals in aviation.
Even if your goals are still to be a major airline pilot (which only means that you haven't been paying attention for the last 7 years), you don't need to go through the regionals to get there.
Flying freight for companies such as Ameriflight, AirNet, Mountain Air Cargo, Empire, etc will provide you with invaluable single-pilot and crew experience flying in the IFR system and making decisions.
Why is that important? We can teach a monkey to manipulate the controls and fly the aircraft... but we can not teach him to be decision maker. We can't teach him when to say "no". We can't teach him that it's ok to go-around. We can't teach him to avoid airframe icing. Get my point?
Those are skills that are developed by flying as PIC in the IFR system. They are also the skills that will make you a valuable resource to the captains you fly with...rather than a liability. Remember that the Captain is NOT your flight instructor (although some of them may act like it). You are a team and if one team member is unqualified, the burden shifts to the other.
I would MUCH rather fly with a first officer who has cut his teeth flying single-pilot into Newark in the middle of the night, then someone who hasn't even given any dual in a C152. It is the difference between knowing that I can count on the fella in the right seat, or spending 4 days watching him like a hawk.
Ok -- now that being said, SOME of these freight operators fly turbine powered, crew aircraft. AirNet has Lears, Empire has the Fairchild, Ameriflight has the B1900 and the EMB120, Air Cargo Carriers has the Shorts 330/360. If your goal is to fly for the majors any of those are EVERY BIT AS VALUABLE as RJ time. In fact, i'd say they may be MORE valuable because it separates you from the pack. It makes your resume stand out among the sea of candidates with the same few thousand hours of RJ time.
And quite frankly, you will be a better pilot then you would sitting there watching the autopilot track the LNAV back to Cincinnati 4 times a day.
As an additional benefit, many of these operators use FBOs where they have the additional possibility of networking with corporate and fractional pilots. So if you are interested in looking at THOSE segments of our profession, there is an opportunity that you wouldn't get strutting through the terminal at JFK...again.
Don't get stuck like a deer in the headlights with only a one-track career mindset. Another 09/11, increased fuel prices, or an accident with a low-timer at the controls could ALL dramatically change the airline landscape and leave you with no "plan B". Trust me. I've been there.
Good luck whatever you choose.